TW201709231A - Sintered body for forming rare-earth magnet, and rare-earth sintered magnet - Google Patents

Sintered body for forming rare-earth magnet, and rare-earth sintered magnet Download PDF

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TW201709231A
TW201709231A TW105109247A TW105109247A TW201709231A TW 201709231 A TW201709231 A TW 201709231A TW 105109247 A TW105109247 A TW 105109247A TW 105109247 A TW105109247 A TW 105109247A TW 201709231 A TW201709231 A TW 201709231A
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magnet
alignment
angle
material particles
rare earth
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TWI674594B (en
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藤川憲一
山本貴士
江部宏史
藤原誠
井本栄一
大牟礼智弘
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日東電工股份有限公司
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    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C38/00—Ferrous alloys, e.g. steel alloys
    • C22C38/005—Ferrous alloys, e.g. steel alloys containing rare earths, i.e. Sc, Y, Lanthanides
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/032—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials
    • H01F1/04—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials metals or alloys
    • H01F1/047—Alloys characterised by their composition
    • H01F1/053—Alloys characterised by their composition containing rare earth metals
    • H01F1/0536—Alloys characterised by their composition containing rare earth metals sintered
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/032—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials
    • H01F1/04—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials metals or alloys
    • H01F1/047—Alloys characterised by their composition
    • H01F1/053—Alloys characterised by their composition containing rare earth metals
    • H01F1/055—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5
    • H01F1/057—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 and IIIa elements, e.g. Nd2Fe14B
    • H01F1/0571—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 and IIIa elements, e.g. Nd2Fe14B in the form of particles, e.g. rapid quenched powders or ribbon flakes
    • H01F1/0575—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 and IIIa elements, e.g. Nd2Fe14B in the form of particles, e.g. rapid quenched powders or ribbon flakes pressed, sintered or bonded together
    • H01F1/0577—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 and IIIa elements, e.g. Nd2Fe14B in the form of particles, e.g. rapid quenched powders or ribbon flakes pressed, sintered or bonded together sintered
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/032—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials
    • H01F1/04—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials metals or alloys
    • H01F1/06—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials metals or alloys in the form of particles, e.g. powder
    • H01F1/068—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials metals or alloys in the form of particles, e.g. powder having a L10 crystallographic structure, e.g. [Co,Fe][Pt,Pd] (nano)particles
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    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F7/00—Magnets
    • H01F7/02—Permanent magnets [PM]
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F2301/00—Metallic composition of the powder or its coating
    • B22F2301/35—Iron
    • B22F2301/355—Rare Earth - Fe intermetallic alloys
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F2304/00—Physical aspects of the powder
    • B22F2304/10—Micron size particles, i.e. above 1 micrometer up to 500 micrometer
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F41/00—Apparatus or processes specially adapted for manufacturing or assembling magnets, inductances or transformers; Apparatus or processes specially adapted for manufacturing materials characterised by their magnetic properties
    • H01F41/02—Apparatus or processes specially adapted for manufacturing or assembling magnets, inductances or transformers; Apparatus or processes specially adapted for manufacturing materials characterised by their magnetic properties for manufacturing cores, coils, or magnets
    • H01F41/0253—Apparatus or processes specially adapted for manufacturing or assembling magnets, inductances or transformers; Apparatus or processes specially adapted for manufacturing materials characterised by their magnetic properties for manufacturing cores, coils, or magnets for manufacturing permanent magnets
    • H01F41/0273—Imparting anisotropy

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  • Crystallography & Structural Chemistry (AREA)
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Abstract

Provided are: a sintered body that forms a rare-earth magnet and is configured in a manner such that the divergence between the orientation angles of the easy axes of magnetization of magnet material particles and the orientation axis angle of the magnet material particles is kept within a prescribed range in an arbitrary micro-section of a magnet cross-section; and a rare-earth sintered magnet. This sintered body for forming a rare-earth magnet has two or more different regions exhibiting an orientation axis angle of at least 20 DEG, given that the orientation axis angle is defined as the highest-frequency orientation angle among the orientation angles of the easy magnetization axes, relative to a pre-set reference line, of a plurality of magnet material particles in a rectangular section at an arbitrary position in a plane including the thickness direction and the widthwise direction. The orientation-angle variance angle is 16.0 DEG or less relative to said orientation axis angle, given that the orientation-angle variance angle is defined on the basis of the difference between the orientation angles of the easy magnetization axes of the magnet material particles. One embodiment defines said section as a rectangular section containing 30 or more magnet material particles, and for example, containing 200 or 300 magnet material particles. It is preferable for the rectangular section to be a square. Another embodiment defines said section as a square section having 35[mu]m sides.

Description

稀土類磁石形成用燒結體及稀土類燒結磁石 Sintered body for rare earth magnet formation and rare earth sintered magnet

本發明係有關用以形成稀土類燒結磁石之稀土類永久磁石形成用燒結體及使該燒結體磁化而得之稀土類磁石。尤其本發明有關具有使含稀土類物質且各具有易磁化軸之多數磁石材料粒子一體燒結而成之構成之稀土類磁石形成用燒結體及使該燒結體磁化而得之稀土類磁石。 The present invention relates to a sintered body for forming a rare earth permanent magnet for forming a rare earth sintered magnet and a rare earth magnet obtained by magnetizing the sintered body. In particular, the present invention relates to a sintered body for forming a rare earth magnet having a structure in which a plurality of magnet material particles each having a rare earth-containing material and having an easy magnetization axis are integrally sintered, and a rare earth magnet obtained by magnetizing the sintered body.

稀土類燒結磁石作為可期待高的保磁力及殘留磁通密度之高性能永久磁石而受到矚目且已實用化，且正進行用以更高性能化之開發。例如日本金屬學會誌第76卷第1期(2012)第12頁至16頁中記載之宇根康也等人之以「藉由結晶微粒化之Nd-Fe-B燒結磁石之高保磁力化」為題之論文(非專利文獻1)記載磁石材料之粒徑若較細則保磁力增大為眾所悉知且已被認知，且為了Nd-Fe-B系燒結磁石之高保磁力化時，記載有使用平均粉末粒徑為1μm之磁石形成用材料粒子進行稀土類燒結磁石之製造之例。該非專利文獻1中記載之稀土類燒結磁石之製造方法中，記載有使磁石材料粒子與由界面活性劑所成之潤滑劑 混合之混合物填充於碳製模具中，將該模具固定於空芯線圈內並施加脈衝磁場，而使磁石材料粒子配向。然而，以該方法，磁石材料粒子之配向由於藉由由空芯線圈所施加之脈衝磁場一概決定，故無法獲得於磁石內之不同位置，使磁石材料粒子於各不同之期望方向配向之永久磁石。且該非專利文獻1中，關於藉由脈衝磁場之施加而配向之磁石材料粒子之易磁化軸是否對於意圖之配向方向會有某程度之偏移之方面、以及其配向角度偏移對磁石性有多少影響之方面均未有任何探討。 The rare earth sintered magnet has been attracting attention as a high-performance permanent magnet that can be expected to have high coercive force and residual magnetic flux density, and has been developed for higher performance. For example, in the Journal of the Japan Society of Metals, Vol. 76, No. 1, (2012), pages 12 to 16, Yu Genkang and others have "high magnetic polarization of Nd-Fe-B sintered magnets by crystal micronization". The paper of the title (Non-Patent Document 1) describes that the particle size of the magnet material is well known and recognized by the increase in the magnetic properties of the magnet, and that the magnetic properties of the Nd-Fe-B sintered magnet are high. An example of producing a rare earth sintered magnet using a material particle for magnet formation having an average powder particle diameter of 1 μm is used. In the method for producing a rare earth sintered magnet described in Non-Patent Document 1, a magnet made of a magnet material particle and a surfactant is described. The mixed mixture is filled in a carbon mold, and the mold is fixed in the hollow core coil and a pulsed magnetic field is applied to align the magnet material particles. However, in this method, the alignment of the magnet material particles is determined by the pulsed magnetic field applied by the air core coil, so that the magnetite material particles can not be obtained at different positions in the magnet, and the magnet material particles are aligned in different desired directions. . Further, in the non-patent document 1, whether the easy magnetization axis of the magnet material particles aligned by the application of the pulse magnetic field has a certain degree of deviation with respect to the intended alignment direction, and the alignment angle shift has a magnetism. There has been no discussion on how much impact.

日本特開平6-302417號公報(專利文獻1)揭示製造以稀土類元素R與Fe及B為基本構成元素之稀土類永久磁石時，以使磁石材料粒子之易磁化軸分別於不同方向配向之複數磁石體接合之狀態下，保持於高溫加熱狀態，藉由此磁石間接著，而形成具有磁石材料粒子之易磁化軸朝不同方向配向之複數區域之永久磁石之方法。依據該專利文獻1中記載之永久磁石形成方法，可能製造於複數區域之各者中，包含易磁化軸以任意且不同方向配向之磁石材料粒子之由複數區域所成之稀土類永久磁石。然而，該專利文獻1中關於賦予至各個磁石體之磁石材料粒子之配向對於意圖之配向方向偏移程度如何之方面未有任何陳述。 Japanese Patent Publication No. 6-302417 (Patent Document 1) discloses a method of producing a rare earth permanent magnet having a rare earth element R and Fe and B as basic constituent elements so that the easy magnetization axes of the magnet material particles are aligned in different directions. In the state in which the plurality of magnet bodies are joined, the method is maintained in a high-temperature heating state, whereby the magnets are connected to each other to form a permanent magnet having a plurality of regions in which the magnetization axis of the magnet material particles are aligned in different directions. According to the permanent magnet forming method described in Patent Document 1, it is possible to manufacture a rare earth permanent magnet formed of a plurality of regions of the magnet material particles in which the magnetization axis is aligned in an arbitrary and different direction, in each of the plurality of regions. However, in Patent Document 1, there is no statement as to how the alignment of the magnet material particles imparted to the respective magnet bodies is to the extent of the intended alignment direction.

日本特開2006-222131號公報(專利文獻2)則揭示於周方向配置偶數個永久磁石片並連結之圓環狀稀土類永久磁石之製造方法。該專利文獻2中所教示之稀土類 永久磁石之製造方法為了形成具有上下扇形主面與一對側面之扇形永久磁石片，而使用具有扇形空腔之粉末加壓裝置，於該扇形空腔內填充稀土類合金粉末，藉由具有配向線圈之上下沖壓，邊對該空腔內之稀土類合金粉末施加配向磁場，邊使該稀土類合金粉末加壓成形者。藉由該步驟，形成於各主面之N極與S極之間具有極向異性之永久磁石片。若詳細描述，則係形成具有自一主面與一側面交叉之角部向另一主面之方向弧狀地彎曲，且於該一主面與另一側面交叉之角部延伸之方向配向之磁化配向之永久磁石片。如此形成之極異向性永久磁石片之偶數個以相鄰永久磁石片成為對向極性之方式連結為圓環狀，獲得圓環狀永久磁石。 Japanese Laid-Open Patent Publication No. 2006-222131 (Patent Document 2) discloses a method of manufacturing an annular rare earth permanent magnet in which an even number of permanent magnet pieces are arranged in the circumferential direction. The rare earths taught in Patent Document 2 Method for manufacturing a permanent magnet In order to form a sector-shaped permanent magnet piece having a vertical main surface and a pair of side surfaces, a powder pressurizing device having a fan-shaped cavity is used, and the fan-shaped cavity is filled with a rare earth alloy powder by having an alignment The coil is pressed up and down, and a rare earth alloy powder is applied to the rare earth alloy powder in the cavity to pressurize the rare earth alloy powder. By this step, permanent magnet pieces having extreme anisotropy between the N pole and the S pole of each main surface are formed. If it is described in detail, it is formed such that a corner portion intersecting from one main surface and one side surface is curved in an arc shape toward the other main surface, and a direction in which the corner portion intersecting the one main surface intersects the other side is aligned. A magnetized permanent magnet piece. An even number of the extremely anisotropic permanent magnet pieces thus formed are connected in an annular shape so that adjacent permanent magnet pieces become opposite in polarity, and a ring-shaped permanent magnet is obtained.

專利文獻2中又記載將連結為圓環狀之偶數個扇狀永久磁石片中，彼此交替配置之磁石片之磁化方向設為軸方向，以成為該等軸方向配向之方式磁化之磁石片之間所配置之磁石片之磁化方向設為徑向之磁石片之排列。以該配置可說明為，交替配置之於軸方向磁化之磁石片之主面之極性互為不同，藉由使於軸方向磁化之磁石片之間配置之於交替配置之徑向磁化之磁石片成為同極相互對向，而使磁通集中於軸方向磁化之一磁石片之一主面之磁極，來自該磁極之磁通可效率良好地集束於於軸方向磁化之另一磁石片之一主面之磁極。然而，該專利文獻2中針對賦予至各個磁石材料粒子之配向對於意圖之配向方向以何種程度偏移之方面亦未有任何描述。 Further, in the case of the even-numbered fan-shaped permanent magnet pieces which are connected in a ring shape, the magnetization direction of the magnet pieces which are alternately arranged in the ring shape is the axial direction, and the magnet pieces are magnetized so as to be aligned in the equiaxed direction. The magnetization direction of the magnet pieces disposed between them is set as the arrangement of the magnet pieces in the radial direction. According to this configuration, the polarities of the main faces of the magnet pieces which are alternately arranged in the axial direction magnetization are different from each other, and the magnet pieces which are magnetized in the axial direction are disposed between the magnet pieces which are alternately arranged in the radial magnetization. The magnetic poles of one of the magnet pieces are magnetized in the axial direction, and the magnetic flux from the magnetic poles can be efficiently bundled in one of the other magnet pieces magnetized in the axial direction. The magnetic pole of the main surface. However, in Patent Document 2, there is no description as to the extent to which the alignment imparted to the respective magnet material particles is shifted to the intended alignment direction.

日本特開2015-32669號公報(專利文獻3)及日本特開平6-244046號公報(專利文獻4)揭示使含稀土類元素R及Fe與B之磁石材料粉末加壓成形，形成平板狀壓粉體，對該壓粉體施加平行磁場進行磁場配向，於燒結溫度進行燒結而形成燒結磁石，接著以不超過燒結溫度之溫度條件，使用按壓部為圓弧狀之模具將該燒結磁石加壓成形為圓弧狀，藉此形成徑向配向之稀土類永久磁石之方向。該專利文獻3中，雖揭示可使用平行磁場形成徑向配向之磁石之方法者，但由於自平板形狀彎曲成為圓弧狀係在磁石材料燒結後進行，故成形困難，不可能進行大的變形或變形為複雜形狀。因此，由該方法可製造之磁石限於該專利文獻4中記載之徑向配向磁石。再者，該專利文獻4針對賦予至各個磁石材料粒子之配向對於意圖之配向方向以何種程度偏移之方面亦未有任何描述。 Japanese Patent Publication No. 2015-32669 (Patent Document 3) and JP-A-6-244046 (Patent Document 4) disclose that a magnet material powder containing a rare earth element R and Fe and B is press-formed to form a flat plate pressure. The powder is subjected to a magnetic field alignment by applying a parallel magnetic field to the green compact, and is sintered at a sintering temperature to form a sintered magnet, and then the sintered magnet is pressed using a mold having an arc-shaped pressing portion at a temperature not exceeding the sintering temperature. Formed into an arc shape, thereby forming the direction of the radially aligned rare earth permanent magnet. In Patent Document 3, a method of forming a magnet in a radial direction by using a parallel magnetic field is disclosed. However, since the shape of the flat plate is curved and the arc shape is formed after the magnet material is sintered, molding is difficult, and large deformation is impossible. Or deformed into a complex shape. Therefore, the magnet which can be manufactured by this method is limited to the radial alignment magnet described in Patent Document 4. Further, this Patent Document 4 does not describe the extent to which the alignment imparted to the respective magnet material particles is shifted to the intended alignment direction.

日本專利第5444630號公報(專利文獻5)揭示嵌入磁石型馬達中使用之平板形狀之永久磁石。該專利文獻5中揭示之永久磁石係於橫剖面內，易磁化軸對於厚度方向之傾斜角度自寬度方向兩端部朝向寬度方向中央部連續變化之徑向配向。若具體陳述，則磁石之易磁化軸以於磁石之橫剖面內自寬度方向中央部朝厚度方向延伸之假想線上之一點集束之方式配向。作為具有此種易磁化軸之徑向配向之永久磁石之製造方法，於專利文獻5中，描述為成形時可以容易實現之磁場配向形成且可容易製造。該專利文獻5中教示之方法於磁石成形時，係施加集束於磁石 外一點之磁場者，且形成之磁石中之易磁化軸之配向限於徑向配向。因此，例如於橫剖面內之寬度方向中央區域成為平行於厚度方向之配向，無法形成易磁化軸配向為於寬度方向兩端部之區域成為斜向配向之永久磁石。該專利文獻5針對賦予至各個磁石材料粒子之配向對於意圖之配向方向以何種程度偏移之方面亦未有任何描述。 Japanese Patent No. 5,446,630 (Patent Document 5) discloses a permanent magnet of a flat plate shape used in a magnet-type motor. The permanent magnet disclosed in Patent Document 5 is in a cross section, and the inclination angle of the easy magnetization axis in the thickness direction is radially aligned from the both end portions in the width direction toward the center portion in the width direction. Specifically, the easy magnetization axis of the magnet is aligned so as to be bundled at one point on the imaginary line extending in the thickness direction from the central portion in the width direction in the cross section of the magnet. As a method of manufacturing a permanent magnet having such a radial alignment of the easy axis of magnetization, Patent Document 5 describes a magnetic field alignment which can be easily realized during molding and which can be easily manufactured. The method taught in Patent Document 5 applies a bundle to a magnet when forming a magnet. The magnetic field of the outer point is, and the alignment of the easy magnetization axis in the formed magnet is limited to the radial alignment. Therefore, for example, the central portion in the width direction in the cross section is aligned in the direction parallel to the thickness direction, and the permanent magnet which is aligned in the direction in which the easy magnetization axis is aligned at both end portions in the width direction is not formed. This Patent Document 5 does not describe any aspect to which the orientation imparted to the respective magnet material particles is shifted with respect to the intended alignment direction.

日本特開2005-44820號公報(專利文獻6)揭示組裝入馬達時實質上不發生齒形力矩(cogging torque)之極異向性稀土類燒結環狀磁石之製造方法。此處揭示之稀土類燒結環狀磁石於周方向空出間隔之複數位置具有磁極，磁化方向於該磁極位置成為法線方向，於鄰接之磁極之中央位置以成為接線方向之方式進行磁化。該專利文獻6中記載之稀土類燒結環狀磁石之製造方法局限於極異向性之磁石製造，以該製造方法，無法製造於單一燒結磁石內，於任意之複數區域內，對磁石材料粒子賦予各不同方向之配向之磁石。且，該專利文獻6針對賦予至各個磁石材料粒子之配向對於意圖之配向方向以何種程度偏移之方面亦未有任何描述。 Japanese Laid-Open Patent Publication No. 2005-44820 (Patent Document 6) discloses a method for producing an extremely anisotropic rare earth sintered annular magnet which does not substantially generate a cogging torque when incorporated in a motor. The rare earth sintered annular magnet disclosed herein has magnetic poles at a plurality of positions spaced apart in the circumferential direction, and the magnetization direction is in the normal direction at the magnetic pole position, and is magnetized so as to be in the wiring direction at the center position of the adjacent magnetic poles. The method for producing a rare earth sintered annular magnet described in Patent Document 6 is limited to the production of an extremely anisotropic magnet, and in this manufacturing method, it is not possible to manufacture the magnet material particles in any of a plurality of regions in a single sintered magnet. A magnet that is assigned to each direction. Further, this Patent Document 6 does not describe the extent to which the alignment imparted to the respective magnet material particles is shifted to the intended alignment direction.

日本特開2000-208322號公報(專利文獻7)揭示於複數區域內具有磁石材料粒子於不同方向配向之構成且為單一板狀的扇形永久磁石。該專利文獻7中，於該永久磁石形成複數區域，於一區域磁石材料粒子配向為平行於厚度方向之圖型，於與其鄰接之其他區域，對於磁石材料粒子賦予對於該一區域之磁石材料粒子之配向方向具有 角度之配向。於專利文獻7中記載為，具有此種磁石材料粒子之配向之永久磁石可採用粉末冶金法，於模具內進行加壓成形時，藉由自配向構件施加適當方向之磁場而製造。然而，該專利文獻7中記載之永久磁石製造方法亦僅能適用於具有特定配向之磁石之製造，所製造之磁石形狀亦受限者。且，該專利文獻7針對賦予至各個磁石材料粒子之配向對於意圖之配向方向以何種程度偏移之方面亦未有任何描述。 Japanese Laid-Open Patent Publication No. 2000-208322 (Patent Document 7) discloses a sector-shaped permanent magnet having a single plate shape in which a plurality of magnet material particles are aligned in different directions in a plurality of regions. In Patent Document 7, in the permanent magnet, a plurality of regions are formed, and in a region, the magnet material particles are aligned in a pattern parallel to the thickness direction, and in other regions adjacent thereto, magnet particles are applied to the magnet material particles for the region. Orientation direction The orientation of the angle. Patent Document 7 discloses that a permanent magnet having such an alignment of the magnet material particles can be produced by a powder metallurgy method, and when a pressure molding is performed in a mold, a magnetic field in an appropriate direction is applied from the alignment member. However, the permanent magnet manufacturing method described in Patent Document 7 can also be applied only to the manufacture of a magnet having a specific alignment, and the shape of the magnet to be produced is also limited. Further, this Patent Document 7 does not describe any aspect to which the orientation imparted to the respective magnet material particles is shifted to the intended alignment direction.

國際申請公開再公表公報WO2007/119393號(專利文獻8)記載將含稀土類元素之磁石材料粒子與結合劑之混合物成形為特性形狀，對該成形體施加平行磁場，對磁石材料粒子產生平行配向，藉由將該成形體變形為其他形狀，而使磁石材料粒子之配向成為非平行之永久磁石之製造方法。該專利文獻8所揭示之磁石具有磁石材料粒子由樹脂組成物結合之構成之所謂黏合磁石，而非燒結磁石。黏合磁石由於具有於磁石材料粒子之間介存樹脂組成物之構造，故與燒結磁石相比成為磁特性差者，無法形成高性能之磁石。 Japanese Patent Laid-Open Publication No. WO2007/119393 (Patent Document 8) discloses that a mixture of a rare earth element-containing magnet material particle and a binder is formed into a characteristic shape, and a parallel magnetic field is applied to the molded body to produce parallel alignment of the magnet material particles. By deforming the formed body into another shape, the alignment of the magnet material particles becomes a method of manufacturing a non-parallel permanent magnet. The magnet disclosed in Patent Document 8 has a so-called bonded magnet in which magnet material particles are combined by a resin composition, instead of a sintered magnet. Since the bonded magnet has a structure in which a resin composition is interposed between the magnet material particles, it has a poor magnetic property as compared with the sintered magnet, and a high-performance magnet cannot be formed.

日本特開2013-191612號公報(專利文獻9)揭示使含稀土類元素之磁石材料粒子與樹脂結合劑混合形成混合物，使該混合物成形為薄片狀作成坯片，藉由對該坯片施加磁場而進行磁場配向，對經磁場配向之坯片進行鍛燒處理使樹脂結合劑分解、飛散，其次於燒成溫度燒結，而形成稀土類燒結磁石之方法。依據該專利文獻9中記載 之方法製造之磁石，係易磁化軸於一方向配向之構成，以該方法，無法製造於單一燒結磁石內對於任意複數區域內之磁石材料粒子賦予各不同方向之配向的磁石。且，該專利文獻9針對賦予至各個磁石材料粒子之配向對於意圖之配向方向以何種程度偏移之方面亦未有任何描述。 Japanese Laid-Open Patent Publication No. 2013-191612 (Patent Document 9) discloses that a rare earth element-containing magnet material particle and a resin binder are mixed to form a mixture, and the mixture is formed into a sheet shape to form a green sheet, and a magnetic field is applied to the green sheet. In the case of magnetic field alignment, a green sheet-aligned green sheet is subjected to calcination treatment to decompose and scatter the resin binder, followed by sintering at a firing temperature to form a rare earth sintered magnet. According to the patent document 9, The magnet produced by the method is a structure in which the easy magnetization axis is aligned in one direction, and in this method, it is impossible to manufacture a magnet in which the magnetite material particles in any of the plurality of regions are aligned in different directions in a single sintered magnet. Further, this Patent Document 9 does not describe any aspect to which the orientation imparted to the respective magnet material particles is shifted with respect to the intended alignment direction.

[先前技術文獻] [Previous Technical Literature] [專利文獻] [Patent Literature]

[專利文獻1]日本特開平6-302417號公報 [Patent Document 1] Japanese Patent Laid-Open No. Hei 6-302417

[專利文獻2]日本特開2006-222131號公報 [Patent Document 2] Japanese Patent Laid-Open Publication No. 2006-222131

[專利文獻3]日本特開2015-32669號公報 [Patent Document 3] Japanese Patent Laid-Open Publication No. 2015-32669

[專利文獻4]日本特開平6-244046號公報 [Patent Document 4] Japanese Patent Laid-Open No. Hei 6-244046

[專利文獻5]日本專利第5444630號公報 [Patent Document 5] Japanese Patent No. 5446630

[專利文獻6]日本特開2005-44820號公報 [Patent Document 6] Japanese Patent Laid-Open Publication No. 2005-44820

[專利文獻7]日本特開2000-208322號公報 [Patent Document 7] Japanese Patent Laid-Open Publication No. 2000-208322

[專利文獻8]國際申請公開再公表公報WO2007/119393號 [Patent Document 8] International Application Publication No. WO2007/119393

[專利文獻9]日本特開2013-191612號公報 [Patent Document 9] Japanese Laid-Open Patent Publication No. 2013-191612

[專利文獻10]美國專利第5705902號說明書 [Patent Document 10] US Patent No. 5,759,902

[專利文獻11]日本特開2013-215021號公報 [Patent Document 11] Japanese Patent Laid-Open Publication No. 2013-215021

[非專利文獻] [Non-patent literature]

[非專利文獻1]日本金屬學會誌第76卷第1期(2012)第12頁至16頁 [Non-Patent Document 1] Journal of the Japan Society of Metals, Vol. 76, No. 1 (2012), pages 12 to 16.

如上述，與稀土類永久磁石之製造有關聯之專利文獻及非專利文獻之任一者，針對磁石剖面內之磁石材料粒子之易磁化軸之配向偏差未有任何描述。本發明人等基於使磁石材料粒子於磁石內之不同位置各於不同期望方向配向之上述文獻記載之稀土類燒結磁石及目前實用化之稀土類燒結磁石中之後述定義驗證配向角之偏差，確認配向角之偏差均大於16°。然而於磁石剖面內之微小區劃內所含之複數磁石材料粒子之易磁化軸配向自意圖之配向方向偏移時，均係若越大則磁石性能越降低。 As described above, any of the patent documents and non-patent documents related to the production of the rare earth permanent magnet does not describe the alignment deviation of the easy magnetization axis of the magnet material particles in the magnet section. The inventors of the present invention confirmed the deviation of the verification alignment angle in the rare earth sintered magnet described in the above-mentioned document and the rare earth sintered magnet which has been put into practical use in the different positions in the magnetite at different positions in the magnet, and the verification verification alignment angle is confirmed. The deviation of the alignment angle is greater than 16°. However, when the easy magnetization axis of the plurality of magnet material particles contained in the micro-division in the magnetite section is shifted from the intended alignment direction, the magnet performance is lowered as the larger the orientation is.

因此，本發明之主要目的係提供以磁石剖面內之任意微小區劃內之各磁石材料粒子之易磁化軸之配向角對於磁石材料粒子配向軸角度之偏移維持在特定範圍內之方式構成之稀土類磁石形成用燒結體及稀土類燒結磁石。換言之，本發明提供過去為存在之新穎具有高精度配向之稀土類燒結磁石及用以形成此磁石之燒結體。尤其本發明可提供具有配向軸角度差20°以上之至少2個區域之稀土類燒結磁石中，磁石剖面內之任意微小區劃內之各磁石材料粒子之易磁化軸之配向角對於磁石材料粒子配向軸角度之偏移維持在特定範圍內之方式構成之稀土類磁石形成用燒結體及稀土類燒結磁石。 Accordingly, it is a primary object of the present invention to provide a rare earth in which the alignment angle of the easy magnetization axes of the respective magnet material particles in any micro-division in the magnetite profile is maintained within a specific range for the deviation of the alignment axis angle of the magnet material particles. A sintered body for magnetite formation and a rare earth sintered magnet. In other words, the present invention provides a rare earth sintered magnet having a high-precision alignment in the past and a sintered body for forming the magnet. In particular, the present invention can provide an alignment angle of an easy magnetization axis of each magnet material particle in any micro-division in a magnet cross section to a magnetite particle alignment in a rare earth sintered magnet having at least two regions having an alignment axis angle difference of 20° or more. A sintered body for forming a rare earth magnet and a rare earth sintered magnet which are configured to maintain a shift in the axial angle within a specific range.

為達成上述目的，本發明之一樣態係提供具有使含有稀土類物質之各具有易磁化軸之多數磁石材料粒子一體燒結之構成之稀土類磁石形成用燒結體。該稀土類磁石形成用燒結體具有長度方向之長度尺寸、於與該長度方向呈直角之橫方向之剖面中之於第1表面與第2表面間之厚度方向之厚度尺寸、對於該厚度方向正交之方向之厚度正交尺寸之立體形狀。該稀土類磁石形成用燒結體進而具有於包含厚度方向與厚度正交方向之面內之任意位置之4邊形區劃內之複數磁石材料粒子之各者之易磁化軸相對於預先決定之基準線之配向角中定義為頻率最高之配向角之配向軸角度差20°以上之至少2個區域。而且，基於該磁石材料粒子之各者之易磁化軸之配向角相對於該配向軸角度之差而決定之配向角偏差角度為16.0°以下。一形態中，該區劃係決定為含有30個以上例如200個或300個磁石材料粒子之4邊形區劃。4邊形區劃較好為正方形。其他實施形態中，該區劃係決定為一邊為35μm之正方形區畫。 In order to achieve the above object, the present invention provides a sintered body for forming a rare earth magnet having a structure in which a plurality of magnet material particles each having a rare magnet material and having an easy magnetization axis are integrally sintered. The sintered body for forming a rare earth magnet has a length dimension in the longitudinal direction, a thickness dimension in a thickness direction between the first surface and the second surface in a cross section perpendicular to the longitudinal direction, and a thickness dimension in the thickness direction. The thickness of the intersecting direction is the three-dimensional shape of the orthogonal dimension. The sintered body for forming a rare earth magnet further has an easy magnetization axis of each of the plurality of magnet material particles in a quadrangular region including an arbitrary position in a plane in which the thickness direction and the thickness are orthogonal to the predetermined reference line. The alignment angle is defined as at least two regions having an alignment angle of the highest frequency and an angle difference of 20° or more. Further, the angle of deviation deviation determined by the difference in the alignment angle of the easy magnetization axis of each of the magnet material particles with respect to the angle of the alignment axis is 16.0 or less. In one form, the zone is determined to be a 4-sided zone containing more than 30 particles, for example 200 or 300 magnet materials. The 4-sided zone is preferably square. In other embodiments, the division is determined to be a square area with a side of 35 μm.

本發明之上述樣態中，磁石材料粒子之平均粒徑較好為5μm以下，更好為3μm以下，特佳為2μm以下。且燒結後之磁石材料粒子之長寬比較好為2.2以下，更好為2以下，又更好為1.8以下。本發明之另一樣態中，提供藉由使上述稀土類磁石形成用燒結體磁化而形成之稀土類燒結磁石。本發明之較佳樣態中，上述立體形狀 係形成為於與長度方向呈直角之橫方向之剖面為梯形之形狀。進而，本發明另一較佳樣態中，上述立體形狀係以具有第1表面及第2表面之兩者形成為具有相同曲率中心之圓弧形狀之圓弧狀剖面之方式，形成與長度方向為直角之橫方向之剖面。 In the above aspect of the invention, the average particle diameter of the magnet material particles is preferably 5 μm or less, more preferably 3 μm or less, and particularly preferably 2 μm or less. Further, the length and width of the magnet material particles after sintering are preferably 2.2 or less, more preferably 2 or less, and still more preferably 1.8 or less. In another aspect of the invention, a rare earth sintered magnet formed by magnetizing the sintered body for forming a rare earth magnet is provided. In a preferred aspect of the invention, the three-dimensional shape The cross section in the lateral direction at right angles to the longitudinal direction is formed in a trapezoidal shape. Further, in another preferred aspect of the present invention, the three-dimensional shape is formed in a longitudinal direction such that the first surface and the second surface are formed into an arcuate cross section having an arc shape having the same center of curvature. It is a cross section in the transverse direction of the right angle.

具有上述構成之本發明之稀土類磁石形成用燒結體由於具有多數磁石材料粒子一體燒結而成之構成，故相比於例如專利文獻8所揭示之黏合磁石，磁石材料粒子之密度大幅提高。因此，藉由使該稀土類磁石形成用燒結體磁化而得之稀土類燒結磁石呈現出對於黏合磁石較不那麼優異之磁石性能。又，由於該燒結體係成為於決定為含有30個以上例如200個或300個磁石材料粒子之4邊形區劃或決定為一邊為35μm之正方形區畫之任意4邊形區劃內之複數磁石材料粒子之易磁化軸之配向角偏差角度收斂於16.0°之較小範圍般之高精度配向，故藉由使該燒結體磁化而得之稀土類燒結磁石成為呈現出比以往之稀土類燒結磁石更優異之磁石性能者。 Since the sintered body for forming a rare earth magnet of the present invention having the above-described configuration has a structure in which a plurality of magnet material particles are integrally sintered, the density of the magnet material particles is greatly improved as compared with, for example, the bonded magnet disclosed in Patent Document 8. Therefore, the rare earth sintered magnet obtained by magnetizing the sintered body for forming a rare earth magnet exhibits a magnet performance which is less excellent than that of the bonded magnet. Further, the sintered system is a plurality of magnetite particles in any quadrilateral division which is determined to be a quadrilateral division containing 30 or more, for example, 200 or 300 magnet material particles, or a square region which is determined to be a square region of 35 μm on one side. Since the angle of deviation of the alignment axis of the easy magnetization axis converges to a high-precision alignment in a small range of 16.0°, the rare earth sintered magnet obtained by magnetizing the sintered body is superior to the conventional rare earth sintered magnet. The magnet performance.

1‧‧‧稀土類永久磁石形成用燒結體 1‧‧‧Sintered body for the formation of rare earth permanent magnets

2‧‧‧上邊 2‧‧‧上上

3‧‧‧下邊 3‧‧‧ below

4、5‧‧‧端面 4, 5‧‧‧ end face

6‧‧‧中央區域 6‧‧‧Central Area

7、8‧‧‧端部區域 7, 8‧‧‧ end area

20‧‧‧電動馬達 20‧‧‧Electric motor

21‧‧‧轉子芯 21‧‧‧Rotor core

21a‧‧‧周面 21a‧‧‧Week

22‧‧‧氣隙 22‧‧‧ Air gap

23‧‧‧定子 23‧‧‧ Stator

23a‧‧‧齒 23a‧‧ teeth

23b‧‧‧磁場線圈 23b‧‧‧Magnetic coil

24‧‧‧磁石***用隙縫 24‧‧‧Magnetic insertion slot

24a‧‧‧直線狀中央部分 24a‧‧‧Linear central part

24b‧‧‧傾斜部分 24b‧‧‧ tilted section

30‧‧‧稀土類磁石 30‧‧‧Rare Earth Magnets

117‧‧‧複合材料 117‧‧‧Composite materials

118‧‧‧支撐基材 118‧‧‧Support substrate

119‧‧‧坯片 119‧‧ ‧ blanks

120‧‧‧狹縫模嘴 120‧‧‧Slot nozzle

123‧‧‧加工用薄片 123‧‧‧Processing sheets

125‧‧‧燒結處理用薄片 125‧‧Sintered sheet

C‧‧‧易磁化軸 C‧‧‧Electronic axis

θ‧‧‧傾斜角 θ‧‧‧Tilt angle

圖1係顯示配向角及配向軸角度之概略圖，(a)係顯示稀土類磁石之磁石材料粒子之易磁化軸之配向一例之橫剖 面圖，(b)係顯示決定各個磁石材料粒子之易磁化軸之「配向角」及「配向軸角度」順序之概略放大圖。 Fig. 1 is a schematic view showing an alignment angle and an alignment axis angle, and (a) is a cross-sectional view showing an alignment of an easy magnetization axis of a magnet material particle of a rare earth magnet. In the plan view, (b) is a schematic enlarged view showing the order of "alignment angle" and "alignment axis angle" of the easy magnetization axes of the respective magnet material particles.

圖2係顯示求出配向角偏差角度之順序之圖表。 Fig. 2 is a graph showing the order in which the angle of deviation of the alignment angle is obtained.

圖3係顯示基於EBSD解析之配向角分佈顯示者，(a)係顯示稀土類磁石之軸方向之立體圖，(b)係顯示由該磁石之中央部與兩端部之EBSD解析所得之極點圖之例，(c)係顯示(a)中之沿A2軸之磁石剖面之配向軸角度。 Fig. 3 is a perspective view showing an alignment angle distribution based on EBSD analysis, (a) showing a perspective view of the axial direction of the rare earth magnet, and (b) showing a pole figure obtained by EBSD analysis of the central portion and both end portions of the magnet. For example, (c) shows the angle of the alignment axis of the magnet section along the A2 axis in (a).

圖4係顯示本發明一實施形態之稀土類磁石形成用燒結體之一例之橫剖面之剖面圖，(a)係顯示全體之剖面圖，(b)係端部之放大圖。 Fig. 4 is a cross-sectional view showing a cross section of an example of a sintered body for forming a rare earth magnet according to an embodiment of the present invention, wherein (a) shows a whole cross-sectional view and (b) shows an enlarged view of an end portion.

圖5係顯示嵌入有本發明一實施形態之稀土類燒結磁石之電動馬達之轉子芯上設置之磁石***用隙縫之一例的轉子部分的剖面圖。 Fig. 5 is a cross-sectional view showing a rotor portion of an example of a magnet insertion slit provided in a rotor core of an electric motor incorporating a rare earth sintered magnet according to an embodiment of the present invention.

圖6係顯示於圖5所示之轉子芯嵌入永久磁石之狀態之轉子部分之端面圖。 Fig. 6 is an end view showing a rotor portion in a state in which the rotor core shown in Fig. 5 is embedded in a permanent magnet.

圖7係可應用本發明之永久磁石之電動馬達之橫剖面圖。 Figure 7 is a cross-sectional view of an electric motor to which the permanent magnet of the present invention can be applied.

圖8係顯示由圖4所示之實施形態之燒結體所形成之稀土類永久磁石中之磁通密度之分佈的圖。 Fig. 8 is a view showing a distribution of magnetic flux density in a rare earth permanent magnet formed by the sintered body of the embodiment shown in Fig. 4.

圖9係顯示本發明一實施形態的圖1所示之永久磁石形成用燒結體之製造步驟的概略圖，(a)~(d)顯示至坯片形成之前之各階段。 Fig. 9 is a schematic view showing a manufacturing procedure of the sintered body for forming a permanent magnet shown in Fig. 1 according to an embodiment of the present invention, and (a) to (d) show stages before the formation of the green sheet.

圖10係顯示本實施形態之磁石材料粒子之易磁化軸配向處理之加工用坯片之剖面圖，(a)顯示磁場施加時之薄 片剖面形狀，(b)顯示磁場施加後實施變形處理之燒結處理用薄片之剖面形狀，(c)顯示將第1成形體彎曲變形為第2成形體之加工步驟。 Fig. 10 is a cross-sectional view showing a green sheet for processing of an easy magnetization axis alignment process of magnet particles of the present embodiment, and (a) shows a thin film when a magnetic field is applied. The cross-sectional shape of the sheet, (b) shows the cross-sectional shape of the sheet for sintering treatment subjected to the deformation treatment after the application of the magnetic field, and (c) shows the processing step of bending and deforming the first molded body into the second molded body.

圖11係顯示鍛燒處理之較佳升溫速度之圖表。 Fig. 11 is a graph showing a preferred temperature increase rate of the calcination treatment.

圖12係顯示本發明其他實施形態且與圖10(a)(b)同樣之圖，(a)係顯示第1成形體，(b)係顯示第2成形體。 Fig. 12 is a view similar to Fig. 10 (a) and (b) showing another embodiment of the present invention, wherein (a) shows a first molded body, and (b) shows a second molded body.

圖13係顯示本發明進而其他實施形態且與圖12(a)(b)同樣之圖，(a)係顯示一樣態之第1成形體，(b)係顯示第2成形體，(c)係顯示其他樣態之第2成形體，(d)係顯示進而其他樣態之第1成形體，(e)係顯示第2成形體，(f)係顯示其他樣態之第2成形體。 Fig. 13 is a view similar to Fig. 12 (a) and (b) showing another embodiment of the present invention, wherein (a) shows the first molded body in the same state, and (b) shows the second molded body, (c) The second molded body of the other form is displayed, (d) shows the first molded body of the other form, (e) shows the second molded body, and (f) shows the second molded body of the other form.

圖14係顯示用以製造徑向配向圓環狀磁石之本發明實施形態之圖，(a)係顯示第1成形體之側視圖，(b)係顯示第2成形體之立體圖，(c)係顯示用以製造軸向配向圓環狀磁石之於與(b)不同方向形成為圓環狀之第2成形體之立體圖。 Figure 14 is a view showing an embodiment of the present invention for producing a radially-oriented annular magnet, wherein (a) shows a side view of the first molded body, (b) shows a perspective view of the second molded body, and (c) A perspective view showing a second molded body formed in an annular shape in a direction different from (b) for producing an axially oriented annular magnet.

圖15係顯示使用由圖14之本實施形態製造之圓環狀磁石形成海爾巴克(Halbach)排列之磁石之例的立體圖。 Fig. 15 is a perspective view showing an example of forming a magnet of a Halbach arrangement using the annular magnet produced by the embodiment of Fig. 14.

圖16係顯示本發明實施例5~9中形成第1成形體所使用之模具之空腔之概略立體圖。 Fig. 16 is a schematic perspective view showing a cavity of a mold used for forming a first molded body in Examples 5 to 9 of the present invention.

圖17係顯示本發明實施例5~9中自第1成形體變形為第2成形體之過程之圖，(a)係顯示第1中間成形體，(b)係顯示第2中間成形體，(c)係顯示第3中間成形體，(d)係顯示第2成形體。 17 is a view showing a process of deforming from a first molded body to a second molded body in the fifth to ninth embodiments of the present invention, wherein (a) shows a first intermediate formed body, and (b) shows a second intermediate formed body; (c) shows a third intermediate formed body, and (d) shows a second formed body.

圖18係顯示本發明實施例5~9之稀土類磁石形成用燒結體中之配向軸角度之分析位置的圖。 Fig. 18 is a view showing the analysis position of the alignment axis angle in the sintered body for forming a rare earth magnet according to Examples 5 to 9 of the present invention.

圖19係顯示用以測定配向軸角度之座標系與基準面之圖。 Fig. 19 is a view showing a coordinate system and a reference plane for measuring the angle of the alignment axis.

以下，針對圖式說明本發明實施形態。於說明實施形態之前，針對用語之定義及配向角之測定進行說明。 Hereinafter, embodiments of the present invention will be described with reference to the drawings. Before describing the embodiment, the definition of the term and the measurement of the alignment angle will be described.

[配向角] [Alignment angle]

配向角意指磁石材料粒子之易磁化軸之方向相對於預定之基準線之角度。 The alignment angle means the angle of the direction of the easy magnetization axis of the magnet material particles with respect to a predetermined reference line.

[配向軸角度] [Alignment axis angle]

係於磁石之特定面內預定之區劃內具有之磁石形成材料粒子之配向角中頻度最高之配向角。本發明中，決定配向軸角度之區劃係設為含有30個以上磁石材料粒子之4邊形區劃或一邊為35μm之正方形區劃。 It is the alignment angle with the highest frequency of the alignment angle of the magnet-forming material particles in the predetermined region in the specific face of the magnet. In the present invention, the division which determines the angle of the alignment axis is a square division including 30 or more magnet material particles or a square division having 35 μm on one side.

圖1中顯示配向角及配向軸角度。圖1(a)係顯示稀土類磁石中之磁石材料粒子之易磁化軸之配向一例之橫剖面圖，該稀土類磁石M具有第1表面S-1、於自該第1表面S-1空出厚度t間隔之位置上之第2表面S-2、及寬度W，於寬度W方向之兩端部形成端面E-1、E-2。 於圖示例中，第1表面S-1與第2表面S-2係相互平行之平坦面，於圖示之橫剖面，該等第1表面S-1及第2表面S-2係以相互平行之2條直線表示。端面E-1成為相對於第1表面S-1於上右方向傾斜之傾斜面，同樣，端面E-2成為相對於第2表面S-2於上左方向傾斜之傾斜面。箭頭B-1概略顯示該稀土類磁石M之寬度方向中央區域之磁石材料粒子之易磁化軸之配向軸方向。相對於此，箭頭B-2概略顯示與端面E-1鄰接之區域中磁石材料粒子之易磁化軸之配向軸方向。同樣地，箭頭B-3概略顯示與端面E-2鄰接之區域中磁石材料粒子之易磁化軸之配向軸方向。 The alignment angle and the alignment axis angle are shown in Figure 1. Fig. 1(a) is a cross-sectional view showing an example of the alignment of the easy magnetization axis of the magnet material particles in the rare earth magnet, the rare earth magnet M having the first surface S-1 and being empty from the first surface S-1 The second surface S-2 and the width W at positions where the thickness t is spaced apart form end faces E-1 and E-2 at both end portions in the width W direction. In the illustrated example, the first surface S-1 and the second surface S-2 are flat surfaces that are parallel to each other. In the cross section shown in the drawing, the first surface S-1 and the second surface S-2 are Two straight lines are shown parallel to each other. The end surface E-1 is an inclined surface that is inclined with respect to the first surface S-1 in the upper right direction. Similarly, the end surface E-2 is an inclined surface that is inclined with respect to the second surface S-2 in the upper left direction. The arrow B-1 schematically shows the direction of the alignment axis of the easy magnetization axis of the magnet material particles in the central portion in the width direction of the rare earth magnet M. On the other hand, the arrow B-2 schematically shows the direction of the alignment axis of the easy magnetization axis of the magnet material particles in the region adjacent to the end surface E-1. Similarly, the arrow B-3 schematically shows the direction of the alignment axis of the easy magnetization axis of the magnet material particles in the region adjacent to the end surface E-2.

「配向軸角度」係以箭頭B-1、B-2、B-3表示之該等配向軸與一基準線之間之角度。基準線可任意設定，但如圖1(a)所示之例般，第1表面S-1之剖面以直線表示時，該第1表面S-1之剖面設為基準線較為便利。圖1(b)係顯示決定各個磁石材料粒子之易磁化軸之「配向角」及「配向軸角度」之順序之概略放大圖。圖1(a)所示之稀土類磁石M之任意部位例如圖1(a)所示之4邊形區劃R於圖1(b)中放大顯示。該4邊形區劃R中包含30個以上例如200個至300個之多數磁石材料粒子P。4邊形區劃中所含之磁石材料粒子之數量越多，測定精度越高，但於30個左右，即可以充分精度測定。各磁石材料粒子P具有易磁化軸P-1。易磁化軸P-1通常不具有方向性，但藉由使磁石材料粒子磁化而可成為具有方向性之向量。圖1(b)中係考慮磁化之預定極性，以對於易磁化軸賦予方 向性之箭頭顯示。 The "alignment axis angle" is an angle between the alignment axes and a reference line indicated by arrows B-1, B-2, and B-3. The reference line can be arbitrarily set. However, when the cross section of the first surface S-1 is indicated by a straight line as in the example shown in Fig. 1(a), it is convenient to use the cross section of the first surface S-1 as the reference line. Fig. 1(b) is a schematic enlarged view showing the order of "alignment angle" and "alignment axis angle" of the easy magnetization axes of the respective magnet material particles. An arbitrary portion of the rare earth magnet M shown in Fig. 1(a), for example, the quadrangular division R shown in Fig. 1(a) is shown enlarged in Fig. 1(b). The quadrilateral division R includes 30 or more, for example, 200 to 300, majority magnet material particles P. The larger the number of magnet material particles contained in the 4-sided division, the higher the measurement accuracy, but at about 30, the accuracy can be measured with sufficient precision. Each of the magnet material particles P has an easy magnetization axis P-1. The easy magnetization axis P-1 generally does not have directivity, but can be made into a directional vector by magnetizing the magnet material particles. Figure 1(b) considers the predetermined polarity of magnetization to give way to the easy axis of magnetization. The directional arrow shows.

如圖1(b)所示，各個磁石材料粒子P之易磁化軸P-1具有該易磁化軸所指向之方向與基準線之間之角度的「配向角」。而且，圖1(b)中所示之4邊形區劃R內之磁石材料粒子P之易磁化軸P-1之「配向角」中，頻度最高之配向角稱為「配向軸角度」B。 As shown in Fig. 1(b), the easy magnetization axis P-1 of each of the magnet material particles P has an "alignment angle" of the angle between the direction in which the easy magnetization axis is directed and the reference line. Further, in the "alignment angle" of the easy magnetization axis P-1 of the magnet material particles P in the quadrangular division R shown in Fig. 1(b), the alignment angle having the highest frequency is referred to as "alignment axis angle" B.

[配向角偏差角度] [Alignment Angle Deviation Angle]

求出任意4邊形區劃中之配向軸角度與針對存在於該區劃內之所有磁石材料粒子之其易磁化軸之配向角之差，該配向角之差的分佈中之半值寬所表示之角度值設為配向角偏差角度。圖2係顯示求出配向角偏差角度之順序的圖表。圖2中，各個磁石材料粒子之易磁化軸之配向角相對於易磁化軸之差△θ之分佈由曲線C表示。縱軸所示之累積頻度最大之位置設為100%，累計頻度為50%之配向角差△θ之值為半值寬。 Finding the difference between the angle of the alignment axis in any quadrilateral division and the alignment angle of the easy magnetization axis of all the magnet material particles present in the division, the half value width in the distribution of the difference of the alignment angles The angle value is set to the angle of deviation of the alignment angle. Fig. 2 is a graph showing the procedure for determining the angle of deviation of the alignment angle. In Fig. 2, the distribution of the difference Δθ of the alignment angle of the easy magnetization axes of the respective magnet material particles with respect to the easy magnetization axis is represented by a curve C. The position where the cumulative frequency shown on the vertical axis is the largest is set to 100%, and the value of the alignment angle difference Δθ of the cumulative frequency of 50% is a half value width.

[配向角之測定] [Measurement of alignment angle]

各個磁石材料粒子P之易磁化軸P-1之配向角可基於掃描電子顯微鏡(SEM)圖像藉由「電子後方散射繞射解析法」(EBSD解析法)求出。用於該解析之裝置有具備Oxford Instruments公司製之EBSD檢測器(AZtecHKL EBSD NordlysNano Integrated)之掃描電子顯微鏡，具備東京都昭島市所在之日本電子股份有限公司製 JSM-70001F或EDAX公司製之EBSD檢測器(Hikari High Speed EBSD Detector)之掃描電子顯微鏡，ZEISS公司製之SUPRA40VP。且，作為藉由外部委託進行EBSD解析之事業體有東京都中央區日本橋所在之JFE技術研發股份有限公司及大阪府茨木市所在之日東分析中心股份有限公司。依據EBSD解析，可求出特定區劃內存在之磁石材料粒子之易磁化軸之配向角及配向軸角度，基於該等值，亦可取得配向角偏差角度。圖3係顯示由EBSD解析法之易磁化軸之配向顯示之一例，圖3(a)係顯示稀土類磁石之軸方向之立體圖，圖3(b)係顯示中央部與兩端部由EBSD解析所得之極點圖之例者。且圖3(c)係顯示沿A2軸之磁石剖面中之配向軸角度。配向軸角度可將磁石材料粒子之易磁化軸配向向量分為於包含A1軸與A2軸之平面中之成分與包含A1軸與A3軸之平面中之成分予以表示。A2軸為寬度方向，A3軸為厚度方向。圖3(b)中央之圖係顯示磁石寬度方向中央中，易磁化軸之配向大致沿A1軸之方向。相對於此，圖3(b)之左圖顯示磁石寬度方向左端部中易磁化軸之配向自下向右上方向沿A1軸-A2軸之面傾斜。同樣地，圖3(b)之右圖顯示磁石寬度方向右端部中易磁化軸之配向自下向左上方向沿A1軸-A2軸之面傾斜。如此配向設為配向向量，示於圖3(c)。 The alignment angle of the easy magnetization axis P-1 of each of the magnet material particles P can be obtained by an "electron backscatter diffraction analysis method" (EBSD analysis method) based on a scanning electron microscope (SEM) image. The apparatus for the analysis includes a scanning electron microscope equipped with an EBSD detector (AZtecHKL EBSD Nordlys Nano Integrated) manufactured by Oxford Instruments, and is manufactured by JEOL Ltd., located in Akishima, Tokyo. Scanning electron microscope of JSM-70001F or EDAX EBSD detector (Hikari High Speed EBSD Detector), SUPRA40VP manufactured by ZEISS. In addition, JFE Technology R&D Co., Ltd., where Nihonbashi is located in Chuo-ku, Tokyo, and Nitto-Analysis Co., Ltd., where Ibaraki City, Osaka Prefecture, are located in the business of EBSD analysis. According to the EBSD analysis, the alignment angle and the alignment axis angle of the easy magnetization axis of the magnet material particles existing in the specific region can be obtained, and based on the values, the alignment angle deviation angle can also be obtained. Fig. 3 is a view showing an alignment display of an easy magnetization axis by the EBSD analysis method, Fig. 3(a) is a perspective view showing the axial direction of the rare earth magnet, and Fig. 3(b) is a view showing the central portion and both end portions being analyzed by EBSD. The example of the resulting pole map. And Figure 3(c) shows the angle of the alignment axis in the magnet section along the A2 axis. The alignment axis angle can be expressed by dividing the easy axis of the magnet material particles into a component in a plane including the A1 axis and the A2 axis and a component in a plane including the A1 axis and the A3 axis. The A2 axis is the width direction and the A3 axis is the thickness direction. The middle view of Fig. 3(b) shows the center of the magnet width direction, and the alignment of the easy magnetization axis is substantially along the A1 axis. On the other hand, the left diagram of FIG. 3(b) shows that the alignment of the easy magnetization axis in the left end portion in the width direction of the magnet is inclined from the lower side to the upper right direction along the A1-axis-A2 axis. Similarly, the right diagram of FIG. 3(b) shows that the alignment of the easy magnetization axis in the right end portion of the magnet width direction is inclined from the lower side to the upper left direction along the A1-axis-A2 axis. Such alignment is set as an alignment vector and is shown in Fig. 3(c).

[結晶方位圖] [Crystal orientation map]

係針對存在於任意區劃內之各個磁石材料粒 子，該磁石材料粒子之易磁化軸相對於垂直於觀察面之軸的傾斜角之圖。該圖可基於掃描電子顯微鏡(SEM)圖像作成。 For each magnet material particle that exists in any zone The graph of the tilt angle of the easy magnetization axis of the magnet material particles with respect to the axis perpendicular to the viewing surface. The map can be made based on a scanning electron microscope (SEM) image.

[較佳實施形態] [Better Embodiment]

以下，針對圖說明本發明實施形態。 Hereinafter, embodiments of the present invention will be described with reference to the drawings.

圖4至圖7中，顯示本發明其他實施形態之稀土類磁石形成用燒結體與組裝有由該燒結體形成之永久磁石之電動馬達之一例。稀土類磁石形成用燒結體1含有Nd-Fe-B系磁石材料作為磁石材料。此處，作為Nd-Fe-B系磁石材料，可舉例為例如以重量百分比計以27.0~40.0wt%之比例含有R(R為包含Y之稀土類元素中之1種或2種以上)，以0.6~2wt%之比例含有B，以60~75wt%之比例含有Fe者。典型上，Nd-Fe-B系磁石材料係以27至40wt%之比例含有Nd，以0.8至2wt%之比例含有B，以60至75wt%之比例含有電解鐵的Fe。該磁石材料中，以提高磁特性為目的，亦可少量含有Dy、Tb、Co、Cu、Al、Si、Ga、Nb、V、Pr、Mo、Zr、Ta、Ti、W、Ag、Bi、Zn、Mg等其他元素。 4 to 7 show an example of an electric motor in which a sintered body for forming a rare earth magnet according to another embodiment of the present invention and a permanent magnet formed of the sintered body are assembled. The sintered body 1 for forming a rare earth magnet contains a Nd—Fe—B based magnet material as a magnet material. Here, the Nd—Fe—B-based magnet material may, for example, contain R (R is one or more of rare earth elements containing Y) in a ratio of 27.0 to 40.0% by weight, B is contained in a ratio of 0.6 to 2 wt%, and Fe is contained in a ratio of 60 to 75 wt%. Typically, the Nd-Fe-B based magnet material contains Nd in a ratio of 27 to 40% by weight, B in a ratio of 0.8 to 2% by weight, and Fe of electrolytic iron in a ratio of 60 to 75% by weight. In the magnet material, for the purpose of improving magnetic properties, a small amount of Dy, Tb, Co, Cu, Al, Si, Ga, Nb, V, Pr, Mo, Zr, Ta, Ti, W, Ag, Bi, Other elements such as Zn and Mg.

若參考圖4(a)，則本實施形態之磁石形成用燒結體1係上述磁石材料之微細粒子一體燒結成形者，具有相互平行之上邊2及下邊3、及左右兩端之端面4、5，該端面4、5設為相對於上邊2及下邊3傾斜之傾斜面而形成。上邊2係對應於第2表面之剖面之邊，下邊3係對 應於第1表面之剖面之邊。端面4、5之傾斜角定義為該端面4、5之延長線4a、5a與上邊2之間之角度θ。較佳之形態中，傾斜角θ為45°至80°，更好為55°至80°。其結果，磁石形成用燒結體1形成為具有上邊2短於下邊3之梯形之寬度方向剖面之形狀。 Referring to Fig. 4 (a), the sintered body for forming a magnet according to the present embodiment is formed by integrally sintering fine particles of the above-mentioned magnet material, and has parallel sides 2 and 3, and end faces 4 and 5 of the left and right ends. The end faces 4 and 5 are formed as inclined faces that are inclined with respect to the upper side 2 and the lower side 3. The upper 2 series corresponds to the side of the section of the second surface, and the lower 3 pairs Should be on the side of the section of the first surface. The inclination angle of the end faces 4, 5 is defined as the angle θ between the extension lines 4a, 5a of the end faces 4, 5 and the upper side 2. In a preferred embodiment, the inclination angle θ is 45° to 80°, more preferably 55° to 80°. As a result, the sintered body 1 for forming a magnet is formed into a shape having a cross section of the upper side 2 shorter than the trapezoidal width direction of the lower side 3.

磁石形成用燒結體1於沿著上邊2及下邊3之寬度方向，具有區分為特定尺寸之中央區域6與兩端部側之端部區域7、8之複數區域。中央區域6中，該區域6中所含之磁石材料粒子係其易磁化軸相對於上邊2及下邊3實質上為直角，成為於平行於厚度方向配向之平行配向。相對於此，端部區域7、8中，該區域7、8所含之磁石材料粒子之易磁化軸相對於厚度方向自下向上，配向方向朝中央區域6方向傾斜，其傾斜角於鄰接於端面4、5之位置係沿該端面4、5之傾斜角θ之角度，於鄰接於中央區域6之位置，相對於該上邊2大致為直角，隨著自鄰接於端面4、5之位置朝中央區域6接近逐漸變大。如此之易磁化軸之配向於圖4(a)中，針對中央區域6之平行配向以箭頭9表示，針對端部區域7、8之傾斜配向以箭頭10表示。關於端部區域7、8之傾斜配向若另外表現，則以使該等區域所含之磁石材料粒子之易磁化軸自上邊2與端面4、5交叉之角部朝向中央部，於與端部區域7、8之寬度方向尺寸對應之特定範圍區域集束之方式配向。該配向結果，於端部區域7、8中，易磁化軸指向上邊2之磁石材料粒子之密度高於中央區域6。本發明之較佳形態 中，以使對應於中央區域6之上邊2之寬度方向尺寸亦即平行長度P與上邊2之寬度方向尺寸L之比，亦即平行率P/L為0.05至0.8，更好為0.2至0.5之方式，決定中央區域6與端部區域7、8之尺寸。該實施形態中，中央區域6與接近端部區域7、8之端面之區域，該等區域中所含之磁石材料粒子之易磁化軸之配向成為配向角度差20°以上者。此處，此種配向稱為「非平行配向」。 The sintered body 1 for magnet formation has a plurality of regions which are divided into a central portion 6 having a specific size and end portions 7 and 8 on both end sides in the width direction of the upper side 2 and the lower side 3. In the central region 6, the magnet material particles contained in the region 6 have substantially the right axis of the easy magnetization axis with respect to the upper side 2 and the lower side 3, and are aligned in parallel with the thickness direction. On the other hand, in the end regions 7, 8, the easy magnetization axis of the magnet material particles contained in the regions 7, 8 is from the bottom to the thickness direction, and the alignment direction is inclined toward the central region 6, and the inclination angle is adjacent to The positions of the end faces 4, 5 are at an angle of the inclination angle θ of the end faces 4, 5, adjacent to the central region 6, at a substantially right angle with respect to the upper edge 2, with respect to the position adjacent to the end faces 4, 5 The central area 6 is gradually getting larger. The orientation of such an easy magnetization axis is shown in Fig. 4(a), the parallel alignment for the central region 6 is indicated by the arrow 9, and the oblique alignment for the end regions 7, 8 is indicated by the arrow 10. When the inclination alignment of the end regions 7 and 8 is expressed separately, the easy magnetization axis of the magnet material particles contained in the regions is directed toward the center portion from the corner portion where the upper side 2 intersects the end faces 4 and 5, and the end portion The width directions of the regions 7 and 8 are aligned in a manner corresponding to the bundle of the specific range regions. As a result of this alignment, in the end regions 7, 8, the magnetite material particles having the easy magnetization axis pointing to the upper side 2 have a higher density than the central region 6. Preferred form of the invention The ratio of the width direction corresponding to the width direction 2 of the upper side 2 of the central region 6, that is, the parallel length P to the width direction dimension L of the upper side 2, that is, the parallel ratio P/L is 0.05 to 0.8, more preferably 0.2 to 0.5. In this manner, the dimensions of the central region 6 and the end regions 7, 8 are determined. In this embodiment, the central region 6 and the region close to the end faces of the end regions 7, 8 have an alignment angle difference of 20 or more in the alignment of the easy magnetization axes of the magnet material particles contained in the regions. Here, such alignment is called "non-parallel alignment".

上述之端部區域7、8中之磁石材料之易磁化軸之配向針對端部區域7於圖4(b)中誇大顯示。圖4(b)中，磁石材料粒子之各易磁化軸C於鄰接於端面4之部分大致沿著該端面4，以該端面4之傾斜角θ傾斜而配向。因此該傾斜角隨著自端部接近中央部而逐漸增加。亦即，磁石材料粒子之易磁化軸C之配向成為自下邊3之側向上邊2集束，易磁化軸C指向上邊2之磁石材料粒子之密度比平行配向時更高。 The alignment of the easy magnetization axes of the magnet materials in the end regions 7, 8 described above is exaggerated for the end regions 7 in Figure 4(b). In Fig. 4(b), the respective easy magnetization axes C of the magnet material particles are substantially aligned along the end surface 4 at a portion adjacent to the end surface 4, and are inclined at an inclination angle θ of the end surface 4. Therefore, the inclination angle gradually increases as the end portion approaches the center portion. That is, the alignment of the easy magnetization axis C of the magnet material particles is bundled from the side of the lower side 3 to the upper side 2, and the density of the magnet material particles whose easy magnetization axis C is directed to the upper side 2 is higher than that in the case of parallel alignment.

圖5係放大顯示適於嵌入藉由使具有上述易磁化軸之配向的磁石形成用燒結體1磁化而形成之稀土類磁石而使用之電動馬達20之轉子芯部分之剖面圖。轉子芯21係以其周面21a介隔氣隙22與定子23對向之方式旋轉自如地配置於該定子23內。定子23於周方向具備空出間隔配設之複數齒23a，於該齒23a捲繞磁場線圈23b。上述之氣隙22形成於各齒23a之端面與轉子芯21之周面21a之間。於轉子芯21形成有磁石***用隙縫24。該隙縫24具有直線狀中央部分24a與自該中央部分 24a之兩端部於轉子芯21之周面21a之方向斜向延伸之一對傾斜部分24b。如由圖6所了解，傾斜部分24b位於其末端部接近轉子芯21之周面21a之位置。 FIG. 5 is a cross-sectional view showing, in an enlarged manner, a rotor core portion of the electric motor 20 used for embedding a rare earth magnet formed by magnetizing the sintered body 1 for magnet formation having the alignment of the easy magnetization axis. The rotor core 21 is rotatably disposed in the stator 23 such that the circumferential surface 21a faces the stator 23 with the air gap 22 interposed therebetween. The stator 23 has a plurality of teeth 23a disposed at intervals in the circumferential direction, and the field coil 23b is wound around the teeth 23a. The air gap 22 described above is formed between the end surface of each of the teeth 23a and the circumferential surface 21a of the rotor core 21. A magnet insertion slit 24 is formed in the rotor core 21. The slit 24 has a linear central portion 24a and a central portion thereof Both ends of the 24a extend obliquely in the direction of the circumferential surface 21a of the rotor core 21 to the inclined portion 24b. As understood from Fig. 6, the inclined portion 24b is located at a position where the end portion thereof is close to the circumferential surface 21a of the rotor core 21.

藉由使具有上述易磁化軸配向之磁石形成用燒結體1磁化而形成之稀土類磁石30***圖5所示之轉子芯21之磁石***用隙縫24之狀態示於圖6。如圖6所示，稀土類永久磁石30係其上邊2朝向外側亦即朝向定子23側之方式，***於轉子芯21中形成之磁石***用隙縫24之直線狀中央部分24a。於比***之磁石30之兩端更外側，留有隙縫24之直線狀中央部分24a之一部分與傾斜部分24b作為空隙部。因此，藉由於轉子芯21之隙縫24中***永久磁石而形成之電動馬達20全體以橫剖面圖示於圖7。 The state in which the rare earth magnet 30 formed by magnetizing the sintered body 1 for magnetizing the magnetization axis having the above-described easy axis of magnetization is inserted into the magnet insertion slit 24 of the rotor core 21 shown in Fig. 5 is shown in Fig. 6. As shown in FIG. 6, the rare earth permanent magnet 30 is inserted into the linear central portion 24a of the magnet insertion slit 24 formed in the rotor core 21 so that the upper side 2 faces the outer side, that is, toward the stator 23. Further than the both ends of the inserted magnet 30, a portion of the linear central portion 24a in which the slit 24 is left and the inclined portion 24b serve as a gap portion. Therefore, the entire electric motor 20 formed by inserting a permanent magnet into the slit 24 of the rotor core 21 is shown in cross section in FIG.

圖8係顯示由上述實施形態形成之稀土類永久磁石30之磁通密度分佈者。如圖8所示，磁石30之兩側端部區域7、8之磁通密度D高於中央區域6之磁通密度E。因此，該磁石30嵌入電動馬達20之轉子芯21而作動時，即使對磁石30之端部作用來自定子23之磁通，亦可抑制磁石30之端部減磁，於磁石30之端部於減磁後亦殘留充分之磁通，而防止馬達20之輸出降低。 Fig. 8 is a view showing a magnetic flux density distribution of the rare earth permanent magnet 30 formed by the above embodiment. As shown in FIG. 8, the magnetic flux density D of the end regions 7, 8 on both sides of the magnet 30 is higher than the magnetic flux density E of the central region 6. Therefore, when the magnet 30 is inserted into the rotor core 21 of the electric motor 20, even if the magnetic flux from the stator 23 acts on the end portion of the magnet 30, the end portion of the magnet 30 can be suppressed from demagnetizing at the end of the magnet 30. A sufficient magnetic flux remains after the demagnetization, and the output of the motor 20 is prevented from being lowered.

[稀土類永久磁石形成用燒結體之製造方法] [Method for Producing Sintered Body for Formation of Rare Earth Permanent Magnet]

其次，針對用以製造圖4至圖8所示之實施形態之稀土類磁石形成用燒結體1之本發明一實施形態之 製造方法參考圖9加以說明。圖9係顯示上述2個實施形態之永久磁石形成用燒結體1之製造步驟之概略圖。 Next, an embodiment of the present invention for producing the sintered body 1 for rare earth magnet formation of the embodiment shown in Figs. 4 to 8 is used. The manufacturing method will be described with reference to FIG. Fig. 9 is a schematic view showing a manufacturing procedure of the sintered body 1 for forming a permanent magnet according to the above two embodiments.

首先，藉習知鑄造法製造由特定分率之Nd-Fe-B系合金所成之磁石材料之錠塊。代表性係銣磁石所使用之Nd-Fe-B系合金具有Nd為30wt%，為電解鐵而較佳之Fe為67wt%，B為1.0wt%之比例含有之組成。其次，將此錠塊使用搗礦機或粉碎機等習知手段粗粉碎至粒徑200μm左右之大小。代替地，將錠塊溶解，藉由漏模澆鑄(strip cast)法製作薄片，以氫解碎法粗粉化。藉此，獲得粗粉碎磁石材料粒子115(參考圖9(a))。 First, an ingot of a magnet material made of a specific fraction of Nd-Fe-B alloy is produced by a conventional casting method. The Nd-Fe-B alloy used for the representative neodymium magnet has a composition in which Nd is 30% by weight, is electrolytic iron, preferably Fe is 67% by weight, and B is 1.0% by weight. Next, the ingot is coarsely pulverized to a size of about 200 μm using a conventional means such as a skimmer or a pulverizer. Instead, the ingot was dissolved, and a sheet was produced by a strip casting method, and coarsely pulverized by a hydrogen disintegration method. Thereby, the coarsely crushed magnet material particles 115 are obtained (refer to FIG. 9(a)).

其次，粗粉碎磁石材料粒子115藉由利用珠粒研磨機116之濕式法或使用噴射研磨機之乾式法等微粉碎。例如使用利用珠粒研磨機116之濕式法之微粉碎係於溶劑中將粗粉碎磁石粒子115微粉碎至特定範圍之粒徑，例如0.1μm至5.0μm，較好平均粒徑為3μm以下，處於於溶劑中使磁石材料粒子分散之狀態(參考圖9(b))。隨後，將濕粉碎後之溶劑中所含之磁石粒子藉由真空乾燥等手段予以乾燥，取出乾燥之磁石粒子(未圖示)。此處，粉碎所用之溶劑種類並未特別限制，可使用異丙醇、乙醇、甲醇等之醇類，乙酸乙酯等之酯類，戊烷、己烷等之低級烴類，苯、甲苯、二甲苯等之芳香族類，酮類、該等之混合物等之有機溶劑或液化氬、液化氮、液化氦等無機溶劑。該情況下，溶劑中較好使用不含氧原子之溶劑。 Next, the coarsely pulverized magnet material particles 115 are finely pulverized by a wet method using a bead mill 116 or a dry method using a jet mill. For example, the finely pulverized magnet particles 115 are finely pulverized in a solvent to a specific range of particle diameters by a wet method using a bead mill 116, for example, 0.1 μm to 5.0 μm, preferably an average particle diameter of 3 μm or less. The state in which the magnet material particles are dispersed in a solvent (refer to FIG. 9(b)). Subsequently, the magnet particles contained in the solvent after the wet pulverization are dried by vacuum drying or the like, and the dried magnet particles (not shown) are taken out. Here, the type of the solvent to be used for the pulverization is not particularly limited, and an alcohol such as isopropyl alcohol, ethanol or methanol, an ester such as ethyl acetate, a lower hydrocarbon such as pentane or hexane, benzene or toluene may be used. An aromatic solvent such as xylene, a ketone, an organic solvent such as a mixture thereof, or an inorganic solvent such as liquefied argon, liquefied nitrogen or liquefied hydrazine. In this case, a solvent containing no oxygen atom is preferably used in the solvent.

另一方面，使用利用噴射研磨機之乾式法之 微粉碎中，粗粉碎之磁石材料粒子115於(a)氧含量為0.5%以下且較好實質上為0%之由氮氣、Ar氣體、He氣體等之惰性氣體所成之氛圍中、或(b)氧含量為0.0001至0.5%之由氮氣、Ar氣體、He氣體等之惰性氣體所成之氛圍中，藉由噴射研磨機微粉碎，成為具有6.0μm以下，例如0.7μm至5.0μm之特定範圍之平均粒徑之微粒子。此處，氧濃度實質上為0%不限定於氧濃度完全為0%之情況，意指亦可含有於微粉表面稍形成氧化被膜之程度的量之氧者。 On the other hand, using a dry method using a jet mill In the fine pulverization, the coarsely pulverized magnet material particles 115 are in an atmosphere of (a) an oxygen gas having an oxygen content of 0.5% or less, preferably substantially 0%, of an inert gas such as nitrogen gas, Ar gas or He gas, or b) an atmosphere having an oxygen content of 0.0001 to 0.5% in an inert gas such as nitrogen gas, Ar gas or He gas, which is finely pulverized by a jet mill to have a specific range of 6.0 μm or less, for example, 0.7 μm to 5.0 μm. The average particle size of the particles. Here, the oxygen concentration is substantially 0%, and is not limited to the case where the oxygen concentration is completely 0%, and means that the oxygen may be contained in an amount to the extent that the oxide film is slightly formed on the surface of the fine powder.

其次，將以珠粒研磨機116等微粉碎之磁石材料成形為期望形狀。為了該磁石材料粒子之成形，準備將如上述微粉碎之磁石材料粒子115與由樹脂材料所成之黏合劑混合之混合物亦即複合材料。作為黏合劑使用之樹脂較好為於構造中不含氧原子且具有解聚合性之聚合物。又，如後述之磁石粒子與黏合劑之複合材料為了可再利用成形為期望形狀時所產生之複合材料之剩餘物，且為了可以加熱複合材料以軟化狀態進行磁場配向，較好使用熱可塑性樹脂作為樹脂材料。具體而言，可較好地使用由以下通式(1)表示之單體形成之1種或2種以上之聚合物或共聚物所成之聚合物。 Next, the magnet material which is finely pulverized by the bead mill 116 or the like is formed into a desired shape. For the formation of the magnet material particles, a composite material in which a mixture of the magnet material particles 115 which are finely pulverized as described above and a binder made of a resin material is mixed is prepared. The resin used as the binder is preferably a polymer which does not contain oxygen atoms in the structure and which has depolymerization property. Further, as a composite material of a magnet particle and a binder which will be described later, in order to re-use the remainder of the composite material which is formed into a desired shape, and in order to heat the composite material to perform magnetic field alignment in a softened state, it is preferred to use a thermoplastic resin. As a resin material. Specifically, a polymer obtained by using one or two or more polymers or copolymers of the monomers represented by the following formula (1) can be preferably used.

(但，R1及R2表示氫原子、低級烷基、苯基或乙烯 基)。 (However, R 1 and R 2 represent a hydrogen atom, a lower alkyl group, a phenyl group or a vinyl group).

相當於上述條件之聚合物有例如異丁烯之聚合物的聚異丁烯(PIB)、異戊二烯之聚合物的聚異戊二烯(異戊二烯橡膠，IR)、1,3-丁二烯之聚合物的聚丁二烯(丁二烯橡膠，BR)、苯乙烯之聚合物的聚苯乙烯、苯乙烯與異戊二烯之共聚物的苯乙烯-異戊二烯嵌段共聚物(SIS)、異丁烯與異戊二烯之共聚物的丁基橡膠(IIR)、苯乙烯與丁二烯之共聚物的苯乙烯-丁二烯嵌段共聚物(SBS)、苯乙烯與乙烯、丁二烯之共聚物的苯乙烯-乙烯-丁二烯-苯乙烯共聚物(SEBS)、苯乙烯與乙烯、丙烯之共聚物的苯乙烯-乙烯-丙烯-苯乙烯共聚物(SEPS)、乙烯與丙烯之共聚物的乙烯-丙烯共聚物(EPM)、乙烯、丙烯與二烯單體共聚合之EPDM、2-甲基-1-戊烯之聚合物的2-甲基-1-戊烯聚合樹脂、2-甲基-1-丁烯之聚合物的2-甲基-1-丁烯聚合樹脂等。且，作為黏合劑中使用之樹脂亦可包含少量之含有氧原子、氮原子之單體之聚合物或共聚物(例如聚甲基丙烯酸丁酯或聚甲基丙烯酸甲酯等)之構成。進而，亦可一部分共聚合不相當於上述通式(1)之單體。即使為該情況，亦可達成本發明之目的。 The polymer corresponding to the above conditions is polyisobutylene (PIB) of a polymer such as isobutylene, polyisoprene (isoprene rubber, IR) of a polymer of isoprene, 1,3-butadiene Polybutadiene (butadiene rubber, BR) of polymer, polystyrene of styrene polymer, styrene-isoprene block copolymer of copolymer of styrene and isoprene ( SIS), butyl rubber (IIR) of a copolymer of isobutylene and isoprene, styrene-butadiene block copolymer (SBS) of styrene and butadiene copolymer, styrene and ethylene, butyl Styrene-ethylene-butadiene-styrene copolymer (SEBS) of copolymer of diene, styrene-ethylene-propylene-styrene copolymer (SEPS) of copolymer of styrene and ethylene, propylene, ethylene and Ethylene-propylene copolymer (EPM) of propylene copolymer, ethylene, propylene and diene monomer copolymerized EPDM, 2-methyl-1-pentene polymer 2-methyl-1-pentene polymerization A 2-methyl-1-butene polymer resin of a resin or a polymer of 2-methyl-1-butene. Further, the resin used as the binder may also contain a small amount of a polymer or copolymer of a monomer containing an oxygen atom or a nitrogen atom (for example, polybutyl methacrylate or polymethyl methacrylate). Further, a part of the copolymerization may not correspond to the monomer of the above formula (1). Even in this case, the object of the present invention can be attained.

又，作為黏合劑中使用之樹脂，為了適當進行磁場配向而期望使用於250℃以下軟化之熱可塑性樹脂，更具體而言為玻璃轉移點或流動起始溫度為250℃以下之熱可塑性樹脂。 Further, the resin used as the binder is preferably a thermoplastic resin which is softened at 250 ° C or lower for more appropriate magnetic field alignment, and more specifically, a thermoplastic resin having a glass transition point or a flow initiation temperature of 250 ° C or lower.

為了於熱可塑性樹脂中分散磁石材料粒子， 期望適量添加分散季(配向潤滑劑)。作為分散劑，期望添加醇、羧酸、酮、醚、酯、胺、亞胺、醯亞胺、醯胺、氰、磷系官能基、磺酸、具有雙鍵或三鍵等不飽和鍵之化合物、及液狀飽和烴化合物中之至少一種。亦可混合該等物質之數種而使用。因此，如後述，於對於磁石材料粒子與黏合劑之混合物亦即複合材料施加磁場使該磁石材料磁場配向時，係以加熱混合物使黏合劑成分軟化之狀態進行磁場配向。 In order to disperse magnet material particles in a thermoplastic resin, It is desirable to add an appropriate amount of the dispersion season (alignment lubricant). As the dispersing agent, it is desirable to add an alcohol, a carboxylic acid, a ketone, an ether, an ester, an amine, an imine, a quinone imine, a guanamine, a cyanide, a phosphorus functional group, a sulfonic acid, or an unsaturated bond having a double bond or a triple bond. At least one of a compound and a liquid saturated hydrocarbon compound. It is also possible to mix several of these substances and use them. Therefore, as will be described later, when a magnetic field is applied to the composite material of the mixture of the magnet material particles and the binder, that is, the magnetic field of the magnet material is aligned, the magnetic field is aligned in a state where the binder component is softened by heating the mixture.

藉由使用滿足上述條件之黏合劑作為於磁石材料粒子中混合之黏合劑，可減低燒結後之稀土類永久磁石形成用燒結體內殘存之碳量及氧量。具體而言，可將燒結後之磁石形成用燒結體內殘存之碳量設為2000ppm以下，更好為1000ppm以下，特佳為500ppm以下。又，可將燒結後之磁石形成用燒結體內殘存之氧量設為5000ppm以下，較好為3000ppm以下，更好為2000ppm以下。 By using a binder that satisfies the above conditions as a binder mixed in the magnet material particles, the amount of carbon and the amount of oxygen remaining in the sintered body for forming a rare earth permanent magnet after sintering can be reduced. Specifically, the amount of carbon remaining in the sintered body for forming a magnet after sintering can be 2,000 ppm or less, more preferably 1,000 ppm or less, and particularly preferably 500 ppm or less. In addition, the amount of oxygen remaining in the sintered body for forming a magnet after sintering can be 5,000 ppm or less, preferably 3,000 ppm or less, more preferably 2,000 ppm or less.

黏合劑之添加量係設為於成形漿料或加熱熔融之複合材料時，以提高作為成形結果所得之成形體之厚度精度之方式，可適當填充磁石材料粒子間之空隙之量。例如黏合劑對於磁石材料粒子與黏合劑之合計量之比例設為1wt%至40wt%，更好2wt%至30wt%，又更好3wt%至20wt%。 When the amount of the binder added is set to be a molded slurry or a composite material which is heated and melted, the amount of voids between the particles of the magnet material can be appropriately filled so as to improve the thickness accuracy of the molded body obtained as a result of the molding. For example, the ratio of the binder to the total amount of the magnet material particles and the binder is set to be 1 wt% to 40 wt%, more preferably 2 wt% to 30 wt%, still more preferably 3 wt% to 20 wt%.

以下實施形態中，以將複合材料暫時成形為製品形狀以外之形狀之成形體之狀態於施加平行磁場之磁場中進行磁石材料粒子之配向，於圖4至圖8所示之實施 形態之情況，於隨後將該成形體成為期望之製品形狀，其次藉由進行燒結處理，而成為例如如圖4(a)所示之梯形形狀般之期望製品形狀之燒結磁石。尤其，以下之實施形態中，將磁石材料粒子與黏合劑所成之混合物亦即複合材料117暫時成形為薄片形狀之坯片成形體(以下稱為「坯片」)後，成為用於配向處理之成形體形狀。將複合材料尤其是成形為薄片形狀時，可採用將例如磁石材料粒子與黏合劑之混合物的複合材料117加熱後成形為薄片形狀之熱熔融塗佈，或將含有磁石材料粒子與黏合劑之混合物的複合材料117放入成形模具中加熱及加壓之方法，或將含有磁石材料粒子與黏合劑及有機溶劑之漿料塗佈於基材上而成形為薄片狀之漿料塗佈等之成形。 In the following embodiment, the alignment of the magnet material particles is performed in a magnetic field in which a parallel magnetic field is applied in a state in which the composite material is temporarily molded into a molded body having a shape other than the product shape, and is implemented in FIGS. 4 to 8 . In the case of the form, the formed body is subsequently formed into a desired product shape, and then, by sintering, a sintered magnet having a desired shape of a product such as a trapezoidal shape as shown in Fig. 4 (a) is formed. In the following embodiments, the composite material 117 which is a mixture of the magnet material particles and the binder is temporarily formed into a sheet-shaped green sheet molded body (hereinafter referred to as a "green sheet"), and is used for alignment treatment. The shape of the formed body. When the composite material is formed into a sheet shape in particular, a composite material 117 such as a mixture of magnet material particles and a binder may be heated to form a hot-melt coating into a sheet shape, or a mixture containing particles of a magnet material and a binder may be used. The composite material 117 is placed in a molding die to be heated and pressurized, or a slurry containing particles of a magnet material and a binder and an organic solvent is applied onto a substrate to form a sheet-like slurry coating or the like. .

以下中，尤其針對使用熱熔融塗佈之坯片成形加以說明，但本發明不限定於該等特定之塗佈法。例如亦可藉由將複合材料117放入成形用模具，邊加熱至室溫~300℃，邊以0.1~100MPa加壓進行成形。該情況下，更具體而言，可採用將加熱至軟化溫度之複合材料117施加射出壓擠壓填充至模具中並成形之方法。 Hereinafter, the green sheet molding using hot melt coating will be specifically described, but the present invention is not limited to the specific coating methods. For example, the composite material 117 may be placed in a molding die and heated to room temperature to 300 ° C to be formed by pressurization at 0.1 to 100 MPa. In this case, more specifically, a method in which the composite material 117 heated to the softening temperature is applied to the extrusion die by extrusion pressure is applied.

如所述，於以珠粒研磨機116等微粉碎之磁石材料粒子中混合黏合劑而製作由磁石材料粒子與黏合劑所成之黏土狀混合物亦即複合材料117。此處，作為黏合劑可使用如上述之樹脂及分散劑之混合物。例如作為樹脂，較好使用由構造中不含氧原子，且具有解聚合性之聚合物所成之熱可塑性樹脂，另一方面，作為分散劑，較好 添加醇、羧酸、酮、醚、酯、胺、亞胺、醯亞胺、醯胺、氰、磷系官能基、磺酸、具有雙鍵或三鍵等不飽和鍵之化合物中之至少一種。又，黏合劑之添加量係設為使如上述添加後之複合材料117中之黏合劑相對於磁石材料粒子與黏合劑之合計量之比率為1wt%至40wt%，更好2wt%至30wt%，又更好為3wt%至20wt%。 As described above, the binder is mixed with the finely pulverized magnet material particles such as the bead mill 116 to prepare a composite 117 which is a clay-like mixture of the magnet material particles and the binder. Here, as the binder, a mixture of the above-mentioned resin and dispersant can be used. For example, as the resin, a thermoplastic resin obtained by a polymer having no deoxidation property and having no oxygen atom in the structure is preferably used. On the other hand, as a dispersing agent, it is preferred. Adding at least one of an alcohol, a carboxylic acid, a ketone, an ether, an ester, an amine, an imine, a quinone imine, a guanamine, a cyanide, a phosphorus functional group, a sulfonic acid, or a compound having an unsaturated bond such as a double bond or a triple bond; . Further, the binder is added in such a ratio that the ratio of the binder in the composite material 117 added as described above to the total amount of the magnet material particles and the binder is from 1% by weight to 40% by weight, more preferably from 2% by weight to 30% by weight. More preferably, it is from 3 wt% to 20 wt%.

此處分散劑之添加量較好根據磁石材料粒子之粒徑加以決定，磁石材料粒子之粒徑越小，推薦添加量越多。具體之添加量，相對於磁石材料粒子100重量份，為0.1重量份至10重量份，較好為0.3重量份至8重量份。添加量少時分散效果小，有配向性降低之虞。且，添加量過多時，有污染磁石材料粒子之虞。添加於磁石材料粒子之分散劑附著於磁石材料粒子表面，獲得分散有磁石材料粒子之黏土狀混合物，並且以後述之磁場配向處理中，以輔助磁石材料粒子旋動之方式作用。其結果，施加磁場時容易進行配向，使磁石粒子之易磁化軸方向於大致同一方向一致，亦即可提高配向度。尤其，於磁石材料粒子中混合黏合劑時，由於粒子表面存在黏合劑，故提高磁場配向處理時之摩擦力，因此有粒子配向性降低之虞，而更提高添加配向潤滑劑之效果。 Here, the amount of the dispersant added is preferably determined according to the particle diameter of the magnet material particles, and the smaller the particle diameter of the magnet material particles, the more the recommended amount is added. The specific addition amount is from 0.1 part by weight to 10 parts by weight, preferably from 0.3 part by weight to 8 parts by weight, per 100 parts by weight of the magnet material particles. When the amount of addition is small, the dispersion effect is small, and the alignment property is lowered. Moreover, when the amount of addition is too large, there is a flaw in the particles of the magnet material. The dispersing agent added to the magnet material particles adheres to the surface of the magnet material particles to obtain a clay-like mixture in which the magnet material particles are dispersed, and acts to assist the magnet material particle swirling in the magnetic field alignment treatment to be described later. As a result, when the magnetic field is applied, the alignment is easily performed, and the easy magnetization axis directions of the magnet particles are aligned in substantially the same direction, whereby the alignment degree can be improved. In particular, when a binder is mixed in the magnet material particles, since the binder is present on the surface of the particles, the frictional force during the magnetic field alignment treatment is improved, so that the particle alignment property is lowered, and the effect of adding the alignment lubricant is further enhanced.

磁石材料粒子與黏合劑之混合較好在氮氣、Ar氣體、He氣體等之惰性氣體所成之氛圍中進行。磁石材料粒子與黏合劑之混合係藉由例如將磁石材料粒子與黏合劑分別投入攪拌機中，以攪拌機攪拌而進行。該情況 下，為了促進混練性亦可進行加熱攪拌。進而，磁石材料粒子與黏合劑之混合亦較好在氮氣、Ar氣體、He氣體等之惰性氣體所成之氛圍中進行。又，尤其於以濕式法粉碎磁石粒子之情況，亦可不自粉碎所用之溶劑取出磁石粒子而將黏合劑添加於溶劑中進行混練，隨後使溶劑揮發，獲得複合材料117。 The mixing of the magnet material particles and the binder is preferably carried out in an atmosphere of an inert gas such as nitrogen, Ar gas or He gas. The mixing of the magnet material particles and the binder is carried out by, for example, putting the magnet material particles and the binder into a mixer and stirring them with a stirrer. The situation Next, heating and stirring may be performed in order to promote kneading. Further, the mixing of the magnet material particles and the binder is preferably carried out in an atmosphere of an inert gas such as nitrogen gas, Ar gas or He gas. Further, in particular, in the case where the magnet particles are pulverized by the wet method, the magnet particles may be taken out from the solvent used for the pulverization, and the binder may be added to the solvent to be kneaded, and then the solvent may be volatilized to obtain the composite material 117.

接著，藉由將複合材料117成形為片狀，作成前述之坯片。採用熱熔融塗佈時，藉由加熱複合材料117使該複合材料117熔融，成為具有流動性之狀態後，塗佈於支撐基材118上。隨後，藉由散熱使複合材料117凝固，於支撐基材118上形成長條片狀之坯片119(參考圖9(d))。此情況下，加熱熔融複合材料117時之溫度，係根據所用之黏合劑種類或量而異，但通常設為50℃至300℃。但，有必要設為比所用之黏合劑之流動起始溫度高之溫度。又，使用漿料塗佈時，於大量溶劑中分散磁石材料粒子與黏合劑及有時為任意之助長配向之添加劑而得之漿料塗佈於支撐基材118上。隨後，藉由乾燥使溶劑揮發，而於支撐基材118上形成長條片狀之坯片119。 Next, the composite material 117 is formed into a sheet shape to form the above-mentioned green sheet. In the case of hot melt coating, the composite material 117 is melted by heating the composite material 117 to be in a fluid state, and then applied to the support substrate 118. Subsequently, the composite material 117 is solidified by heat dissipation, and a long sheet-like green sheet 119 is formed on the support substrate 118 (refer to Fig. 9 (d)). In this case, the temperature at which the molten composite material 117 is heated varies depending on the type or amount of the binder to be used, but is usually 50 ° C to 300 ° C. However, it is necessary to set a temperature higher than the flow initiation temperature of the binder used. Further, when the slurry is applied, the slurry obtained by dispersing the magnet material particles and the binder in a large amount of the solvent and the additive which may be any of the assisted alignment may be applied to the support substrate 118. Subsequently, the solvent is volatilized by drying to form a long sheet-like green sheet 119 on the support substrate 118.

此處，熔融之複合材料117之塗佈方式較好使用狹縫模嘴方式或軋光輥方式等之層厚控制性優異之方式。尤其為了實現高的厚度精度，期望使用層厚控制性尤其優異亦即可於基材表面塗佈高精度厚度之層之方式的模嘴方式或缺角輪塗佈方式。例如以狹縫模嘴方式，將加熱而處於具有流動性之狀態之複合材料117藉由齒輪泵壓送 而注入模嘴中，自模嘴噴出而進行塗佈。且，以軋光輥方式，將複合材料117以控制之量送入經加熱之2根輥之捏夾間隙中，邊使輥旋轉邊於支撐基材118上，塗佈以輥之熱熔融之複合材料117。作為支撐基材118，較好使用例如聚矽氧處理之聚酯薄膜。再者，藉由使用消泡劑或進行加熱真空脫泡，以使塗佈並展開之複合材料117之層中不殘留氣泡之方式，進行充分之脫泡處理。或者，並非塗佈於支撐基材118上，而藉由擠出成形或射出成形使熔融之複合材料117成形為薄片狀，邊擠出於支撐基材118上，亦可於支撐基材118上成形坯片119。 Here, the coating method of the molten composite material 117 is preferably a method in which the layer thickness controllability such as the slit die method or the calender roll method is excellent. In particular, in order to achieve high thickness precision, it is desirable to use a nozzle method or a notch wheel coating method in which a layer thickness control property is particularly excellent, that is, a layer of a high-precision thickness can be applied to a surface of a substrate. For example, in a slit die method, the composite material 117 which is heated and in a fluid state is pumped by a gear pump. Injecting into the nozzle, the film is ejected from the nozzle and coated. Further, in a calender roll manner, the composite material 117 is fed into the nip gap of the heated two rolls in a controlled amount, and the roll is rotated on the support substrate 118 to be coated with the hot melt of the roll. Composite material 117. As the support substrate 118, for example, a polyfluorene-treated polyester film is preferably used. Further, by using an antifoaming agent or heating and vacuum defoaming, a sufficient defoaming treatment is performed so that no bubbles remain in the layer of the coated and unrolled composite material 117. Alternatively, instead of being applied to the support substrate 118, the molten composite material 117 is formed into a sheet shape by extrusion molding or injection molding, and extruded on the support substrate 118, or on the support substrate 118. The green sheet 119 is formed.

圖9所示之實施形態中，使用狹縫模嘴120進行複合材料117之塗佈。藉由該狹縫模嘴方式之坯片119之形成步驟中，期望實際測量塗佈後之坯片119之薄片厚度，藉由基於該實測值之反饋控制，而調節狹縫模嘴120與支撐基材118之間之捏夾間隙。該情況中，極力減低供給至狹縫模嘴120之流動性複合材料117之量之變動，例如抑制於±0.1%以下之變動，進而亦使塗佈速度之變動極力降低，例如抑制於±0.1%以下之變動。藉由如此控制，可提高坯片119之厚度精度。又，所形成之坯片119之厚度精度，相對於例如1mm之設計值，較好設為±10%以內，更好設為±3%以內，又更好設為±1%以內。於軋光輥方式，同樣基於實測值反饋控制軋光條件，可控制轉印於支撐基材118之複合材料117之膜厚。 In the embodiment shown in Fig. 9, the coating of the composite material 117 is performed using the slit die 120. In the step of forming the green sheet 119 of the slit die method, it is desirable to actually measure the sheet thickness of the coated green sheet 119, and the slit die 120 and the support are adjusted by feedback control based on the measured value. The pinch gap between the substrates 118. In this case, the fluctuation of the amount of the fluid composite material 117 supplied to the slit die 120 is reduced as much as possible, for example, by a variation of ±0.1% or less, and the fluctuation of the coating speed is also extremely reduced, for example, by ±0.1. % below changes. By thus controlling, the thickness precision of the green sheet 119 can be improved. Further, the thickness accuracy of the formed green sheet 119 is preferably within ±10%, more preferably within ±3%, and even more preferably within ±1%, with respect to a design value of, for example, 1 mm. In the calender roll method, the calendering conditions are also controlled based on the measured value feedback, and the film thickness of the composite material 117 transferred to the support substrate 118 can be controlled.

坯片119之厚度期望設定於0.05mm至20mm 之範圍。厚度若薄於0.05mm，則為了達成必要之磁石厚度，而必須進行多層積層，故而使生產性降低。 The thickness of the green sheet 119 is desirably set to 0.05 mm to 20 mm. The scope. When the thickness is thinner than 0.05 mm, it is necessary to laminate a plurality of layers in order to achieve a necessary magnet thickness, so that productivity is lowered.

其次，自藉由上述之熱熔融塗佈而於支撐基材118上形成之坯片119切出對應於期望磁石尺寸之尺寸作成加工用薄片123。該加工用薄片123係對應於第1成形體者，其形狀與期望之磁石形狀不同。若詳細描述，則該第1成形體之加工用薄片123，於對該加工用薄片123施加平行磁場，使該加工用薄片123中所含之磁石材料粒子之易磁化軸成為平行地配向後，使該加工用薄片123變形成為期望磁石形狀時，針對具有該期望形狀之磁石，成形為能獲得期望易磁化軸之非平行配向之形狀。 Next, the processing sheet 123 is formed by cutting out a size corresponding to the desired magnet size from the green sheet 119 formed on the support substrate 118 by the above-described hot melt coating. The processing sheet 123 corresponds to the first molded body, and its shape is different from the desired magnet shape. In the processing sheet 123 of the first molded body, a parallel magnetic field is applied to the processing sheet 123, and the easy magnetization axes of the magnet material particles contained in the processing sheet 123 are aligned in parallel. When the processing sheet 123 is deformed into a desired magnet shape, the magnet having the desired shape is shaped so as to obtain a non-parallel alignment of the desired easy magnetization axis.

圖4至圖8所示之實施形態中，第1成形體的加工用薄片123係如圖10(a)所示，具有與成為最終製品之梯形剖面之稀土類永久磁石形成用燒結體1之中央區域6對應之寬度方向較長之直線狀區域6a與連續於該直線狀區域6a兩端之圓弧狀區域7a、8a之剖面形狀。該加工用薄片123具有與圖之紙面呈直角方向之長度尺寸，剖面之尺寸及寬度尺寸係預估於後述之燒結步驟中尺寸縮小，而決定為可於燒結步驟後獲得特定之磁石尺寸。 In the embodiment shown in FIG. 4 to FIG. 8 , the processing sheet 123 of the first molded body has the sintered body 1 for forming a rare earth permanent magnet which is a trapezoidal cross section of the final product as shown in FIG. 10( a ). The central region 6 corresponds to a linear region 6a having a long width direction and a cross-sectional shape of the arc-shaped regions 7a and 8a continuous at both ends of the linear region 6a. The processing sheet 123 has a length dimension in a direction perpendicular to the paper surface of the drawing, and the size and width dimension of the cross section are estimated to be reduced in size in a sintering step to be described later, and it is determined that a specific magnet size can be obtained after the sintering step.

對圖10(a)所示之加工用薄片123，以與直線狀區域6a表面呈直角之方向施加平行磁場121。藉由該磁場施加，加工用薄片123所含之磁石材料粒子之易磁化軸如圖10(a)之箭頭122所示，於磁場方向亦即平行於厚度方向配向。 The processing sheet 123 shown in Fig. 10 (a) is applied with a parallel magnetic field 121 in a direction perpendicular to the surface of the linear region 6a. By the application of the magnetic field, the easy magnetization axis of the magnet material particles contained in the processing sheet 123 is aligned in the direction of the magnetic field, that is, parallel to the thickness direction, as indicated by an arrow 122 in Fig. 10(a).

該步驟中，將加工用薄片123收容於具有與該加工用薄片123對應形狀之空腔之磁場施加用模具內(未圖示)，藉由加熱使加工用薄片123中所含之黏合劑軟化。藉此，磁石材料粒子可於黏合劑內旋動，可使其易磁化軸沿平行磁場121之方向高精度地配向。 In this step, the processing sheet 123 is housed in a magnetic field applying mold (not shown) having a cavity corresponding to the processing sheet 123, and the adhesive contained in the processing sheet 123 is softened by heating. . Thereby, the magnet material particles can be rotated in the binder, and the easy magnetization axis can be aligned with high precision in the direction of the parallel magnetic field 121.

此處，用以加熱加工用薄片123之溫度及時間係隨所用之黏合劑種類及量而異，但設為例如於40至250℃歷時0.1至60分鐘。總之，為了使加工用薄片內之黏合劑軟化，加熱溫度必須設為所用黏合劑之玻璃轉移點或流動起始溫度以上之溫度。用以加熱加工用薄片之手段，有例如藉由加熱板之加熱或使用如矽油之熱介質為熱源之方式。磁場施加中之磁場強度可設為5000[Oe]~150000[Oe]，較好為10000[Oe]~120000[Oe]。其結果，加工用薄片123中所含之磁石材料粒子之結晶之易磁化軸如於圖10(a)中符號122所示，於沿平行磁場121之方向平行配向。於該磁場施加步驟中，亦可構成為對於複數個加工用薄片同時施加磁場。為此，只要使用具有複數個空腔之模具或者排列複數個模具同時施加平行磁場121即可。對加工用薄片施加磁場之步驟，可與加熱步驟同時進行，亦可進行加熱步驟後且使加工用薄片內之黏合劑凝固之前進行。 Here, the temperature and time for heating the processing sheet 123 vary depending on the type and amount of the binder to be used, but it is, for example, from 40 to 250 ° C for 0.1 to 60 minutes. In summary, in order to soften the binder in the processing sheet, the heating temperature must be set to a temperature above the glass transition point or the flow initiation temperature of the binder used. The means for heating the processing sheet may be, for example, a heating source or a heat medium such as eucalyptus oil as a heat source. The magnetic field strength in the application of the magnetic field can be set to 5000 [Oe] ~ 150000 [Oe], preferably 10000 [Oe] ~ 120000 [Oe]. As a result, the easy magnetization axes of the crystals of the magnet material particles contained in the processing sheet 123 are aligned in the direction parallel to the parallel magnetic field 121 as indicated by reference numeral 122 in Fig. 10(a). In the magnetic field application step, the magnetic field may be simultaneously applied to a plurality of processing sheets. For this reason, it is only necessary to apply a parallel magnetic field 121 while using a mold having a plurality of cavities or arranging a plurality of dies. The step of applying a magnetic field to the processing sheet may be performed simultaneously with the heating step, or may be performed after the heating step and before the binder in the processing sheet is solidified.

其次，將藉由圖10(a)所示之磁場施加步驟使磁石材料粒子之易磁化軸以箭頭122所示般平行配向之加工用薄片123自磁場施加用模具取出，移至圖10(b)(c)所 示之具有細長之長度方向尺寸之梯形空腔124之最終成形用模具126內，藉由具有與該空腔124對應之凸型形狀之公模127將該加工用薄片123於空腔124內擠壓，而變形為加工用薄片123之兩端部之圓弧狀區域7a、8a對於中央直線狀區域6a直線狀連續，成形為圖10(b)所示之燒結處理用薄片125。該燒結處理用薄片125對應於第2成形體。 Next, the processing sheet 123 in which the easy magnetization axis of the magnet material particles are aligned in parallel as indicated by the arrow 122 is taken out from the magnetic field application mold by the magnetic field application step shown in Fig. 10 (a), and is moved to Fig. 10 (b). ) (c) The final forming mold 126 having a trapezoidal cavity 124 having an elongated longitudinal dimension is extruded in the cavity 124 by a male mold 127 having a convex shape corresponding to the cavity 124. The arc-shaped regions 7a and 8a which are deformed into the both end portions of the processing sheet 123 are linearly continuous with respect to the central linear region 6a, and are formed into the baking treatment sheet 125 shown in Fig. 10(b). This sintering treatment sheet 125 corresponds to the second molded body.

藉由該成形，使加工用薄片123成為兩端之圓弧狀區域7a、8a對於中央直線狀區域6a直線狀連續之形狀，同時於兩端部形成有傾斜面125a、125b，構成細長梯形形狀。藉由該成形步驟所形成之燒結處理用薄片125中，中央直線狀區域6a中所含之磁石材料粒子之易磁化軸維持於與厚度方向平行配向之平行配向狀態，但於兩端區域7a、8a中，向上凸之形狀變形為連續於中央直線狀區域之直線形狀之結果，如圖10(b)所示，易磁化軸於分別對應之區域之上邊集束地配向。 By this molding, the processing sheet 123 has the arc-shaped regions 7a and 8a at both ends linearly continuous with respect to the central linear region 6a, and the inclined surfaces 125a and 125b are formed at both end portions to form an elongated trapezoidal shape. . In the sintering treatment sheet 125 formed by the molding step, the easy magnetization axis of the magnet material particles contained in the central linear region 6a is maintained in a parallel alignment state parallel to the thickness direction, but in the both end regions 7a, In 8a, as a result of the upward convex shape being deformed into a linear shape continuous with the central linear region, as shown in Fig. 10 (b), the easy magnetization axes are bundled and aligned on the respective corresponding regions.

如此使磁石材料粒子之易磁化軸配向之配向後之燒結處理用薄片125被送至鍛燒步驟。鍛燒步驟中之鍛燒處理係於調節為大氣壓或比大氣壓高的壓力或低的壓力例如0.1MPa至70MPa，較好1.0Pa或1.0MPa之非氧化性氛圍中，以黏合劑分解溫度保持數小時至數十小時例如5小時而進行鍛燒處理。於該處理，推薦使用氫氣氛圍或氫與惰性氣體之混合氣體氛圍。藉由氫氣氛圍中進行鍛燒處理時，鍛燒中之氫供給量設為例如5L/min。藉由進行 鍛燒處理，可使黏合劑中所含之有機化合物藉由解聚合反應、其他反應而分解為單體，並飛散去除。亦即，進行可使燒結處理用薄片125中殘存之碳量減低之處理的脫碳處理。且鍛燒處理期望以使燒結處理用薄片125內殘存之碳量成為2000ppm以下，更好1000ppm以下之條件進行。藉此，以隨後之燒結處理可使燒結處理用薄片125全體緻密燒結，可抑制殘留磁通密度及保磁力降低。又，進行上述鍛燒處理時之加壓條件設為高於大氣壓之壓力時，壓力期望為15MPa以下。此處，加壓條件若為高於大氣壓之壓力，更具體而言為0.2MPa以上，則尤其可期待殘存碳量減輕效果。 The sintering treatment sheet 125 after the alignment of the easy magnetization axes of the magnet material particles is sent to the calcination step. The calcination treatment in the calcining step is carried out in a non-oxidizing atmosphere adjusted to atmospheric pressure or a pressure higher than atmospheric pressure or a low pressure, for example, 0.1 MPa to 70 MPa, preferably 1.0 Pa or 1.0 MPa, in which the binder decomposition temperature is maintained. The calcination treatment is carried out for hours to tens of hours, for example, 5 hours. For this treatment, it is recommended to use a hydrogen atmosphere or a mixed gas atmosphere of hydrogen and an inert gas. When the calcination treatment is carried out in a hydrogen atmosphere, the amount of hydrogen supplied during calcination is, for example, 5 L/min. By doing In the calcination treatment, the organic compound contained in the binder can be decomposed into monomers by depolymerization reaction or other reaction, and dispersed and removed. In other words, the decarburization treatment for reducing the amount of carbon remaining in the sintering treatment sheet 125 is performed. In addition, it is desirable to carry out the calcination treatment so that the amount of carbon remaining in the sintering treatment sheet 125 is 2,000 ppm or less, more preferably 1,000 ppm or less. Thereby, the entire sintering processing sheet 125 can be densely sintered by the subsequent sintering treatment, and the residual magnetic flux density and the coercive force can be suppressed from being lowered. Moreover, when the pressurization condition at the time of the said calcination process is set to the pressure higher than atmospheric pressure, it is desirable that the pressure is 15 MPa or less. Here, if the pressurization condition is a pressure higher than atmospheric pressure, more specifically 0.2 MPa or more, the residual carbon amount reducing effect can be expected in particular.

黏合劑分解溫度雖根據黏合劑種類而異，但鍛燒處理溫度若為200℃至900℃，更好300℃至500℃，例如450℃即可。 The decomposition temperature of the binder varies depending on the type of the binder, but the calcination treatment temperature is 200 ° C to 900 ° C, more preferably 300 ° C to 500 ° C, for example, 450 ° C.

上述鍛燒處理中，與一般之稀土類磁石之燒結處理比較，較好升溫速度小。具體而言，藉由使升溫速度設為2℃/min以下，例如1.5℃/min，可獲得較佳結果。因此，進行鍛燒處理時，藉由如圖11所示之2℃/min以下之特定升溫速度升溫，於到達預先設定之設定溫度亦即黏合劑分解溫度後，於該設定溫度保持數小時至數十小時而進行鍛燒處理。如此，藉由此鍛燒處理中之升溫速度減小，不會使燒結處理用薄片125內之碳急遽去除，而可階段性去除，故可使殘留碳減少至充分等級，可使燒結後之永久磁石形成用燒結體之密度上升。亦即，藉由減少殘 留碳量而可減少永久磁石中之空隙。如上述，升溫速度若設為2℃/min左右，則可使燒結後之永久磁石形成用燒結體之密度成為98%以上例如7.40g/cm3以上，更好為7.45g/cm3以上，又更好為7.50g/cm3以上，其結果，可期待於磁化後之磁石中達成高的磁石特性。 In the above calcination treatment, the temperature rise rate is preferably small as compared with the sintering treatment of a general rare earth magnet. Specifically, a preferable result can be obtained by setting the temperature increase rate to 2 ° C / min or less, for example, 1.5 ° C / min. Therefore, when the calcination treatment is performed, the temperature is raised by a specific temperature increase rate of 2 ° C/min or less as shown in FIG. 11 , and after reaching the preset set temperature, that is, the binder decomposition temperature, the temperature is maintained at the set temperature for several hours. The calcination treatment is carried out for several tens of hours. In this way, the temperature increase rate in the calcination treatment is reduced, and the carbon in the sintering treatment sheet 125 is not removed, but can be removed stepwise. Therefore, the residual carbon can be reduced to a sufficient level, and the sintered carbon can be removed. The density of the sintered body for forming a permanent magnet increases. That is, the voids in the permanent magnet can be reduced by reducing the amount of residual carbon. When the temperature rise rate is about 2 ° C / min, the density of the sintered body for forming a permanent magnet after sintering can be 98% or more, for example, 7.40 g/cm 3 or more, more preferably 7.45 g/cm 3 or more. More preferably, it is 7.50 g/cm 3 or more, and as a result, high magnet characteristics can be expected to be achieved in the magnet after magnetization.

接著，進行將藉由鍛燒處理而鍛燒之燒結處理用薄片125燒結之燒結處理。作為燒結處理，亦可採用真空中之無加壓燒結法，但此處說明之實施形態中，較好採用使燒結處理用薄片125於與圖10之紙面垂直之方向的燒結處理用薄片125之長度方向單軸加壓之狀態燒結之單軸加壓燒結法。以該方法，將各燒結處理用薄片125裝填於具有與圖10(b)之符號「124」所示者相同梯形形狀剖面之空腔之燒結用模具(未圖示)內，關閉模具，邊於與圖10之紙面垂直之方向的燒結處理用薄片125之長度方向加壓邊進行燒結。若詳細描述，則係使用將自燒結處理用薄片125形成之稀土類永久磁石，於收容於圖5所示之磁石***用隙縫24時與轉子芯21之軸方向同方向之方向，將燒結處理用薄片125於長度方向加壓之狀態燒結之單軸加壓燒結。作為該加壓燒結技術，亦可採用例如熱加壓燒結、熱靜水壓加壓(HIP)燒結、超高壓合成燒結、氣體加壓燒結、放電電漿(SPS)燒結等之習知技術之任一者。尤其較好使用可於單軸方向加壓之熱加壓燒結。又，以加熱板燒結進行燒結時，較好加壓壓力設為例如0.01MPa~100MPa，於數Pa以下之真空氛圍中以例如3℃/分鐘 ~30℃/分鐘，例如10℃/分鐘之升溫速度使溫度上升至900℃~1000℃，例如940℃，隨後保持至以加壓方向每10秒之變化率成為0為止。該保持時間通常為5分鐘左右。接著冷卻，再次升溫至300℃~1000℃，於該溫度保持2小時進行熱處理。此燒結處理之結果，自燒結處理用薄片125製造本發明之稀土類永久磁石形成用燒結體1。如此，依據使燒結處理用薄片125於長度方向加壓之狀態燒結之單軸加壓燒結法，可抑制對燒結處理用薄片125內之磁石材料粒子賦予之易磁化軸之配向紊亂。於該燒結階段，燒結處理用薄片125內之樹脂材料幾乎全部蒸散，殘存樹脂量即便有亦成為非常微量。 Next, a sintering treatment for sintering the sintering treatment sheet 125 calcined by the calcination treatment is performed. As the sintering treatment, a pressureless sintering method in a vacuum may be employed. However, in the embodiment described herein, the sintering treatment sheet 125 is preferably used for the sintering treatment sheet 125 in the direction perpendicular to the paper surface of Fig. 10 . Uniaxial pressure sintering method in the state of uniaxial pressing in the longitudinal direction. In this method, each of the sintering treatment sheets 125 is placed in a sintering mold (not shown) having a cavity having the same trapezoidal cross section as the one shown by the symbol "124" in Fig. 10(b), and the mold is closed. Sintering is performed while pressing in the longitudinal direction of the sheet 125 for sintering treatment in the direction perpendicular to the sheet surface of Fig. 10 . As described in detail, the rare earth permanent magnet formed from the sheet 125 for sintering treatment is used in the direction of the same direction as the axial direction of the rotor core 21 when being accommodated in the slit 24 for magnet insertion shown in FIG. The uniaxial pressure sintering is performed by sintering the sheet 125 in a state of being pressed in the longitudinal direction. As the pressure sintering technique, conventional techniques such as hot press sintering, hot hydrostatic pressure (HIP) sintering, ultrahigh pressure synthetic sintering, gas pressure sintering, and discharge plasma (SPS) sintering may be employed. Either. It is particularly preferable to use a hot press sintering which can be pressurized in a uniaxial direction. Further, when the hot plate is sintered and sintered, the pressure is preferably 0.01 MPa to 100 MPa, for example, 3 ° C / min in a vacuum atmosphere of several Pa or less. The temperature rise rate of ~30 ° C /min, for example 10 ° C / min, raises the temperature to 900 ° C ~ 1000 ° C, for example 940 ° C, and then maintains until the rate of change in the pressurization direction every 10 seconds becomes zero. This hold time is usually about 5 minutes. Subsequently, the mixture was cooled, heated again to 300 ° C to 1000 ° C, and kept at this temperature for 2 hours for heat treatment. As a result of the sintering treatment, the sintered body 1 for forming a rare earth permanent magnet of the present invention is produced from the sheet 125 for sintering treatment. In the uniaxial pressure sintering method in which the sintering treatment sheet 125 is pressed in the longitudinal direction, the alignment disorder of the easy magnetization axis imparted to the magnet material particles in the sintering treatment sheet 125 can be suppressed. At the sintering stage, almost all of the resin material in the sintering treatment sheet 125 is evaporated, and the amount of residual resin is extremely small even if it is present.

又，藉由燒結處理，使樹脂經蒸散之狀態之前述磁石材料粒子彼此燒結形成燒結體。典型上，藉由燒結處理，使前述磁石材料粒子中之稀土類濃度高的富含稀土類相熔融，埋填前述磁石材料粒子間存在之空隙，形成由具有R2Fe14B組成(R係包含釔之稀土類元素)之主相與富含稀土類相所成之緻密燒結體。 Further, by the sintering treatment, the magnet material particles in a state in which the resin is evaporated are sintered to each other to form a sintered body. Typically, the rare earth-rich phase having a high rare earth concentration in the magnet material particles is melted by sintering treatment, and a void existing between the magnet material particles is buried to form a rare earth containing R2Fe14B (R system containing lanthanum) The main phase of the class element) and the dense sintered body formed by the rare earth-rich phase.

圖示實施形態之情況，稀土類永久磁石形成用燒結體1以未磁化之狀態***圖5所示之轉子芯21之磁石***用隙縫24內。隨後，對於***該隙縫24內之稀土類永久磁石形成用燒結體1，以沿著其中所含之磁石材料粒子之易磁化軸亦即C軸進行磁化。若具體描述，則對於***轉子芯21之複數隙縫24之複數稀土類永久磁石形成用燒結體1，以沿著轉子芯21之周方向，交替配置N 極與S極之方式進行磁化。其結果，可製造永久磁石1。又，稀土類永久磁石形成用燒結體1磁化時，可使用例如磁化線圈、磁化軛、電容式磁化電源裝置等之習知手段之任一者。又，亦可在稀土類永久磁石形成用燒結體1***隙縫24之前進行磁化，作成稀土類永久磁石，再將該磁化之磁石***隙縫24中。 In the case of the embodiment, the rare earth permanent magnet forming sintered body 1 is inserted into the magnet insertion slit 24 of the rotor core 21 shown in Fig. 5 in an unmagnetized state. Subsequently, the sintered body 1 for forming a rare earth permanent magnet inserted into the slit 24 is magnetized along the axis of easy magnetization of the magnet material particles contained therein. Specifically, for the plurality of rare earth permanent magnet forming sintered bodies 1 inserted into the plurality of slits 24 of the rotor core 21, N is alternately arranged along the circumferential direction of the rotor core 21. The magnetization is performed in the manner of the pole and the S pole. As a result, the permanent magnet 1 can be manufactured. Further, when the sintered body 1 for rare earth permanent magnet formation is magnetized, any of conventional means such as a magnetization coil, a magnetization yoke, and a capacitive magnetization power supply device can be used. Further, the rare earth permanent magnet forming sintered body 1 may be magnetized before being inserted into the slit 24 to form a rare earth permanent magnet, and the magnetized magnet may be inserted into the slit 24.

依據上述說明之稀土類永久磁石形成用燒結體之製造方法，藉由使磁石材料粒子與黏合劑混合之混合物的複合材料成形，藉由邊加熱至超過複合材料之軟化點之溫度邊自外部對加工用薄片施加平行磁場，可使易磁化軸以高精度於期望方向配向。因此可防止配向方向之偏差，亦可提高磁石性能。再者，由於使與黏合劑之混合物成形，故與使用壓粉成形等之情況比較，配向後磁石粒子亦不會旋動，可進一步提高配向度。依據對於磁石材料粒子與黏合劑之混合物的複合材料施加磁場進行配向之方法，由於可適當增加使用於形成磁場之電流通過之捲線匝數，故可確保進行磁場配向時之磁場強度增大，且可以靜磁場長時間施加磁場，故可實現偏差少之高配向度。而且，若如圖5至圖9所示之實施形態般，於配向後修正配向方向之方式，則可確保高配向且偏差少的配向。 According to the method for producing a sintered body for forming a rare earth permanent magnet according to the above description, the composite material of the mixture of the magnet material particles and the binder is formed by heating to a temperature exceeding the softening point of the composite material from the outside. By applying a parallel magnetic field to the processing sheet, the easy magnetization axis can be aligned with a high precision in a desired direction. Therefore, the deviation of the alignment direction can be prevented, and the performance of the magnet can be improved. Further, since the mixture with the binder is molded, the magnet particles are not rotated after the alignment, and the degree of alignment can be further improved. According to the method of aligning a magnetic field applied to a composite material of a mixture of a magnet material particle and a binder, since the number of winding turns for passing a current for forming a magnetic field can be appropriately increased, the magnetic field strength at the time of magnetic field alignment can be ensured to be increased, and The magnetic field can be applied for a long time in a static magnetic field, so that a high degree of alignment with less variation can be achieved. Further, as in the embodiment shown in FIGS. 5 to 9, the alignment direction is corrected after the alignment, and the alignment with high alignment and small variation can be ensured.

如此，所謂可實現偏差少之高配向度與減低燒結所致之收縮偏差有關。因此，可確保燒結後之製品形狀之均一性。其結果，減輕了對於燒結後之外形加工之負擔，可期待大幅提高量產之安定性。又，於磁場配向之步 驟中，對於磁石粒子與黏合劑之混合物的複合材料施加磁場，並且於圖5至圖9所示之實施形態之情況下，藉由使經施加磁場之複合材料朝最終形狀之成形體變形，而操作易磁化軸之方向，進行磁場配向。因此藉由使暫時經磁場配向之複合材料變形，可修正配向方向，以使易磁化軸朝向減磁對象區域適當集束之方式配向。其結果，即使賦予複雜配向時，亦可達成高配向且偏差少的配向。 Thus, the high degree of alignment in which the deviation can be achieved is related to the reduction of the shrinkage deviation due to sintering. Therefore, the uniformity of the shape of the product after sintering can be ensured. As a result, the burden on the external processing after sintering is alleviated, and the stability of mass production can be expected to be greatly improved. Again, in the direction of magnetic field alignment In the step, a magnetic field is applied to the composite material of the mixture of the magnet particles and the binder, and in the case of the embodiment shown in FIGS. 5 to 9, by deforming the composite material to which the magnetic field is applied toward the final shaped body, In the direction of the easy magnetization axis, the magnetic field alignment is performed. Therefore, by deforming the composite material temporarily aligned by the magnetic field, the alignment direction can be corrected so that the easy magnetization axis is aligned so as to be appropriately bundled toward the demagnetization target region. As a result, even when a complex alignment is imparted, an alignment with a high alignment and a small variation can be achieved.

如此所得之稀土類磁石形成用燒結體中，配向角偏差角度可設為16.0°以下，較好設為14.0°以下，更好設為12.0°以下，又更好設為10.0°以下。藉由使配向角偏差角度成為該範圍，可提高殘留磁通密度。 In the sintered body for forming a rare earth magnet obtained in this manner, the angle of deviation of the alignment angle can be 16.0 or less, preferably 14.0 or less, more preferably 12.0 or less, still more preferably 10.0 or less. By making the angle of deviation of the alignment angle into this range, the residual magnetic flux density can be increased.

又，如此所得之稀土類磁石形成用燒結體中，由於易磁化軸可以高精度於期望方向配向，故可成為具有配向軸角度差20°以上之至少2個區域者。此處，配向軸角度係參考圖1(a)(b)如前所述，係定義為於包含厚度方向與於厚度正交之寬度方向之稀土類永久磁石形成用燒結體剖面內之任意位置所決定之於包含30個以上磁石材料粒子之4鞭刑區劃內之所有磁石材料粒子之各者之易磁化軸相對於預定之基準線之配向角中頻度最高之配向角。該配向軸角度之差較好為25°以上，更好為為30°以上，又更好為為35°以上，特佳為為40°以上。 Further, in the sintered body for forming a rare earth magnet obtained in this manner, since the easy magnetization axis can be aligned with a high precision in a desired direction, it is possible to have at least two regions having an alignment axis angle difference of 20 or more. Here, the angle of the alignment axis is defined as any position in the cross section of the sintered body for forming a rare earth permanent magnet including the thickness direction and the width direction orthogonal to the thickness, as described above with reference to Fig. 1 (a) and (b). It is determined that the susceptibility angle of the easy magnetization axis of each of the magnet material particles in the four whip divisions including the 30 or more magnet material particles is the highest among the alignment angles of the predetermined reference line. The difference in the angle of the alignment axis is preferably 25 or more, more preferably 30 or more, still more preferably 35 or more, and particularly preferably 40 or more.

再者，前述2個區域係選擇為其中心間之直線距離d為15mm以下，該等2個區域中所求出之配向軸角度之差較好為15°以上，更好為為20°以上，又更好為 25°以上。此處，前述2個區域更好選擇為其距離d為10mm以下，又更好為5mm以下。具體而言，較好選擇為前述d成為8mm。 Further, the two regions are selected such that the linear distance d between the centers is 15 mm or less, and the difference between the alignment axis angles obtained in the two regions is preferably 15 or more, more preferably 20 or more. And better 25° or more. Here, the above two regions are preferably selected such that the distance d is 10 mm or less, and more preferably 5 mm or less. Specifically, it is preferred to select that the above d is 8 mm.

且，一般稀土類永久磁石形成用燒結體由於有接近表面之區域配向紊亂之傾向，以排除其影響為目的，為了求出配向軸角度之差所選擇之前述2個區域較好以該區域於自最接近之表面至少遠離0.5mm之位置分別選擇，更好於至少遠離0.7mm之位置分別選擇。 In addition, in general, a sintered body for forming a rare earth permanent magnet has a tendency to be disordered in a region close to the surface, and for the purpose of eliminating the influence thereof, the two regions selected to obtain the difference in the angle of the alignment axis are preferably the region. It is selected from the position where the closest surface is at least 0.5 mm away, and is better selected at least at a position away from 0.7 mm.

圖12(a)(b)係顯示本發明方法之其他實施形態且與圖10(a)(b)同樣之圖。如圖12(a)所示，自坯片119形成之第1成形體200係由一對腳部200a、200b與該腳部200a、200b之間之半圓形部分200c所成之倒U字形狀，該第1成形體200中之磁石材料粒子之易磁化軸藉由外部平行磁場之施加而成為如圖12(a)之箭頭200d所示，於圖之自左至右方向平行配向。該U字形狀之第1成形體200以特定溫度條件變形，成為圖12(b)所示之成形為直線狀之第2成形體201。自第1成形體200朝第2成形體201之變形較好以不產生不合理變形之方式逐次階段進行。因此，較好準備具有與各變形階段之形狀對應之空腔之成形用模具，於該成形用模具內進行成形。圖12(b)所示之第2成形體201中，該第2成形體201之磁石材料粒子之易磁化軸，於一端之端部區域201a係成為如圖中箭頭202所示自圖之上指向下之平行配向，於另一端之端部區域201b係成為如圖中箭頭203所示自圖之下指向上之平行 配向。於兩端部區域201a、201b之間之中央區域201c，係成為如圖中箭頭204所示朝上凹入的半圓形配向。藉由將使該第2成形體201燒結所得之稀土類磁石形成用燒結體磁化而形成之稀土類永久磁石，產生自一端之端部區域201b之上面流出磁石外，沿著圓弧狀路徑，自另一端之端部區域201a之上面進入磁石內之磁通流動。因此，依據該磁石，可於磁石之單面生成增強之磁通流動，可獲得例如適於線性馬達使用之永久磁石。 Fig. 12 (a) and (b) are views similar to Fig. 10 (a) and Fig. 10 (b) showing another embodiment of the method of the present invention. As shown in Fig. 12(a), the first molded body 200 formed from the green sheet 119 is an inverted U-shaped word formed by the pair of leg portions 200a and 200b and the semicircular portion 200c between the leg portions 200a and 200b. The shape of the magnetization axis of the magnet material particles in the first molded body 200 is as shown by an arrow 200d in Fig. 12(a) by the application of an external parallel magnetic field, and is aligned in parallel from the left to the right in the drawing. The U-shaped first molded body 200 is deformed under specific temperature conditions, and becomes the second molded body 201 which is formed into a linear shape as shown in Fig. 12(b). The deformation from the first molded body 200 to the second molded body 201 is preferably performed in a stepwise manner so as not to cause unreasonable deformation. Therefore, it is preferable to prepare a molding die having a cavity corresponding to the shape of each deformation stage, and to perform molding in the molding die. In the second molded body 201 shown in Fig. 12(b), the easy magnetization axis of the magnet material particles of the second molded body 201 is formed on the end portion 201a at one end as shown by an arrow 202 in the figure. Pointing to the parallel alignment, the end region 201b at the other end is parallel to the top from the bottom of the figure as indicated by arrow 203 in the figure. Orientation. The central region 201c between the end portions 201a and 201b is a semicircular alignment that is recessed upward as indicated by an arrow 204 in the figure. The rare earth permanent magnet formed by magnetizing the sintered body for forming a rare earth magnet obtained by sintering the second molded body 201 is generated from the upper surface of the end portion 201b of one end and flows out of the magnet along the arcuate path. The magnetic flux flows into the magnet from the upper end of the end portion 201a at the other end. Therefore, according to the magnet, an enhanced magnetic flux flow can be generated on one side of the magnet, and a permanent magnet suitable for use in a linear motor can be obtained, for example.

圖13(a)係顯示本發明其他實施形態者，第1成形體300與圖12(a)之第1成形體200中之倒U字形狀比較，係成為一對腳部300a、300b於與半圓形部分300c相反側之端部向寬度方向打開之形狀。因此，平行磁場之施加方向於圖中自下指向上。因此，第1成形體300中所含之磁石材料粒子之易磁化軸如圖13(a)之箭頭300d所示，自下向上平行配向。該第1成形體300變形為圖13(b)所示之圓弧狀，成為第2成形體300e。該第2成形體300e中所含之磁石材料粒子之易磁化軸300f如圖13(b)所示，隨著朝向寬度方向之中央部，配向角逐漸增大，成為朝向中央部集束之配向。如此，可形成具有用於極異向配向之圓弧狀片段磁石之易磁化軸配向的燒結體。圖13(c)係圖13(b)之變形，第2成形體300g係自第1成形體300變形為細長之長方體形狀。該變化例之第2成形體300g中之易磁化軸300h之配向成為與圖13(b)所示同樣者。使圖13(b)所示之極異向配向之圓弧狀片段燒結形 成之燒結體磁化所得之極異向配向之圓弧狀片段磁石於周方向並排配置於電動馬達之轉子周面，於構成永久磁石表面配置型馬達(SPM馬達)中使用。 Fig. 13 (a) shows another embodiment of the present invention, in which the first molded body 300 is compared with the inverted U shape in the first molded body 200 of Fig. 12 (a), and is formed as a pair of leg portions 300a and 300b. The end of the opposite side of the semicircular portion 300c is opened in the width direction. Therefore, the direction in which the parallel magnetic field is applied is directed downward from the figure. Therefore, the easy magnetization axis of the magnet material particles contained in the first molded body 300 is parallel-aligned from the bottom to the top as indicated by an arrow 300d in Fig. 13(a). The first molded body 300 is deformed into an arc shape as shown in FIG. 13(b) to form a second molded body 300e. As shown in Fig. 13 (b), the easy magnetization axis 300f of the magnet material particles contained in the second molded body 300e gradually increases in the alignment direction toward the center portion in the width direction, and becomes an alignment toward the center portion. In this way, a sintered body having an easy axis of alignment of the arc-shaped segment magnets for extremely anisotropic alignment can be formed. Fig. 13 (c) is a modification of Fig. 13 (b), and the second molded body 300g is deformed from the first molded body 300 into a long rectangular parallelepiped shape. The alignment of the easy magnetization axis 300h in the second molded body 300g of this modification is the same as that shown in Fig. 13(b). Sintering the arc-shaped segment of the extremely anisotropic alignment shown in Fig. 13(b) The arc-shaped segment magnets of the extremely anisotropic alignment obtained by magnetization of the sintered body are arranged side by side in the circumferential direction on the rotor circumferential surface of the electric motor, and are used in a permanent magnet surface-arranged type motor (SPM motor).

圖13(d)係顯示藉由將圖13(a)所示之第1成形體300上下反轉，形成為具有一對腳部400a、400b與該腳部400a、400b間之半圓形部分400c之開腳U字形之第1成形體400者。外部平行磁場係於圖中由下指向上。其結果，該第1成形體400中所含之磁石材料粒子之易磁化軸如圖中以符號400d所示，成為自下指向上之平行配向。藉由將該第1成形體400變形為具有比半圓形部分400之曲率半徑大之曲率半徑的圓弧狀而形成之第2成形體400e示於圖13(e)。該第2成形體400e中所含之磁石材料粒子之易磁化軸400f如圖13(e)所示，成為自寬度方向中央部向端部擴展之配向。圖13(f)為圖13(e)之變形，第2成形體400g係自第1成形體400變形為細長長方體形狀而成。該變形例之第2成形體400g中之易磁化軸400h之配向成為與圖13(e)所示相同者。 Fig. 13 (d) shows a semicircular portion having a pair of leg portions 400a and 400b and the leg portions 400a and 400b formed by vertically inverting the first molded body 300 shown in Fig. 13(a). The first molded body 400 of the U-shaped opening of the 400c. The external parallel magnetic field is directed from the bottom to the top in the figure. As a result, the easy magnetization axis of the magnet material particles contained in the first molded body 400 is parallel alignment from the lower direction as indicated by reference numeral 400d in the drawing. The second molded body 400e formed by deforming the first molded body 400 into an arc shape having a curvature radius larger than the radius of curvature of the semicircular portion 400 is shown in Fig. 13(e). As shown in Fig. 13 (e), the easy magnetization axis 400f of the magnet material particles contained in the second molded body 400e is aligned from the central portion in the width direction to the end portion. Fig. 13 (f) is a modification of Fig. 13 (e), and the second molded body 400 g is deformed from the first molded body 400 into an elongated rectangular parallelepiped shape. The alignment of the easy magnetization axis 400h in the second molded body 400g of this modification is the same as that shown in Fig. 13(e).

圖14(a)(b)係顯示製造圓環狀且磁石材料粒子之易磁化軸配向於半徑方向之徑向配向之稀土類磁石形成用燒結體之方法的側視圖及立體圖。圖14(a)係顯示第1成形體500者，該第1成形體500係具有第1表面的下面500a、平行於該下面500a之第2表面的上面500b、與兩端之端面500c、500d之大致長方形橫剖面，且係具有與圖之紙面成直角方向之長度之長方體形狀。對該第1成形 體500施加自下向上之平行外部磁場，使該第1成形體500中所含之磁石材料粒子之易磁化軸如圖14(a)以符號500e所示般，自下面500a朝向上面500b平行配向。該第1成形體500係於圖14(a)之紙面之平面內，以上面500b為外側，以下面500a為內側之方式彎曲為圓環狀。該彎曲加工時，以使兩端面500c、500d適當對接形成圓環之方式，將該兩端面斜向切斷。因此，對接之兩端面500c、500d相互熔合接合。藉由該彎曲加工及兩端部之熔合而形成圖14(b)所示之圓環狀之第2成形體500g。如圖14(b)所示，第2成形體500g中，磁石材料粒子之易磁化軸500f成為半徑方向之徑向配向。其次，若參考圖14(c)，則圖14(a)所示之第1成形體500以使與圖之紙面直角之方向亦即長度方向延伸之部分成為內側之方式，彎曲為圓環狀。該情況下，以彎曲加工時使兩端面500c、500d適當對接而形成圓環之方式，將該兩端面於長度方向斜向切斷。因此，對接之兩端面500c、500d相互熔合接合。藉由該彎曲加工及兩端部之熔合而形成圖14(c)所示之圓環狀之第2成形體500g'。如圖14(c)所示，第2成形體500g'中，磁石材料粒子之易磁化軸500h成為與圓環之軸方向平行之軸向配向。 (a) and (b) of FIG. 14 are a side view and a perspective view showing a method of producing a sintered body of a rare earth magnet for forming an annular shape in which an easy magnetization axis of a magnet material particle is aligned in a radial direction. Fig. 14 (a) shows a first molded body 500 having a lower surface 500a of a first surface, an upper surface 500b parallel to a second surface of the lower surface 500a, and end faces 500c and 500d at both ends. It has a substantially rectangular cross section and has a rectangular parallelepiped shape having a length in a direction perpendicular to the paper surface of the drawing. The first forming The body 500 is applied with a parallel external magnetic field from the bottom to the top, and the easy magnetization axis of the magnet material particles contained in the first molded body 500 is aligned in parallel from the lower surface 500a toward the upper surface 500b as shown by reference numeral 500e in Fig. 14(a). . The first molded body 500 is formed in a plane of the paper surface of Fig. 14(a), and is curved in an annular shape with the upper surface 500b being the outer side and the lower surface 500a being the inner side. In the bending process, the end faces 500c and 500d are alternately butted to form a ring, and the both end faces are obliquely cut. Therefore, the butted end faces 500c, 500d are fused to each other. The annular second molded body 500g shown in Fig. 14(b) is formed by the bending process and the fusion of both end portions. As shown in Fig. 14 (b), in the second molded body 500g, the easy magnetization axis 500f of the magnet material particles is radially aligned in the radial direction. Then, referring to Fig. 14 (c), the first molded body 500 shown in Fig. 14 (a) is curved in a ring shape so that a portion extending in a direction perpendicular to the direction perpendicular to the plane of the drawing, that is, a longitudinal direction is formed inside. . In this case, the end faces 500c and 500d are appropriately butted together to form a ring shape during the bending process, and the both end faces are cut obliquely in the longitudinal direction. Therefore, the butted end faces 500c, 500d are fused to each other. The annular second molded body 500g' shown in Fig. 14(c) is formed by the bending process and the fusion of both end portions. As shown in Fig. 14 (c), in the second molded body 500g', the easy magnetization axis 500h of the magnet material particles is aligned in the axial direction parallel to the axial direction of the ring.

圖15顯示使圖14(b)所示之形成為徑向配向之圓環狀之第2成形體500g與圖14(c)所示之形成為軸向配向之圓環狀之第2成形體500g’燒結之稀土類磁石形成用燒結體磁化而得之燒結型稀土類永久磁石互相交互重疊 而形成之海爾巴克排列之磁石。海爾巴克排列之圓環狀磁石可望用於同步線性馬達等之用途，例如美國專利第5705902號說明書(專利文獻10)中揭示將此種磁石使用於直列電動發電機之例，於日本特開2013-215021號公報(專利文獻11)中雖揭示其他應用例，但以安定且低廉價格製造徑向配向及軸向配向之圓環磁石並不容易。然而，依據本發明之方法，如上述可容易地製造高磁特性之徑向及軸向配向圓環狀磁石。 Fig. 15 shows a second molded body 500g having an annular shape formed in a radial direction as shown in Fig. 14(b) and a second molded body formed in an annular shape as shown in Fig. 14(c). 500g' sintered rare earth magnets are formed by sintering a sintered body to obtain sintered rare earth permanent magnets which overlap each other The formation of the Heilbach array of magnets. The ring magnet of the Herbak array is expected to be used for a synchronous linear motor or the like. For example, an example of using such a magnet for an in-line motor generator is disclosed in Japanese Patent No. 5,590,902 (Patent Document 10). Although other application examples are disclosed in Japanese Patent Publication No. 2013-215021 (Patent Document 11), it is not easy to manufacture a ring-shaped magnet having a radial alignment and an axial alignment at a stable and inexpensive price. However, according to the method of the present invention, the radial and axial alignment annular magnets of high magnetic properties can be easily fabricated as described above.

如上述之稀土類磁石形成用燒結體藉由將其磁化，可不限於以往習知之非平行配向磁石，而可形成具有任意配向及形狀之磁石。因此，本實施形態之稀土類磁石形成用燒結體，於較佳形態，可成為具有與用以形成磁石粒子全部徑向配向之環形狀之磁石的徑向環磁石形成用燒結體不同之配向或形狀之稀土類磁石形成用燒結體。更佳之形態，係可成為具有與用以形成該徑向環狀磁石及磁石粒子全部係極異向性配向之環形狀之磁石之燒結體不同之配向或形狀之稀土類磁石形成用燒結體。 The sintered body for forming a rare earth magnet as described above can be magnetized, and can be formed into a magnet having an arbitrary alignment and shape without being limited to the conventional non-parallel alignment magnet. Therefore, in the preferred embodiment, the sintered body for forming a rare earth magnet of the present embodiment may have an orientation different from that of a sintered body for forming a radial ring magnet for forming a magnet having a ring shape in which all of the magnet particles are aligned in the radial direction. A sintered body for forming a rare earth magnet of a shape. A more preferable form is a sintered body for forming a rare earth magnet having an alignment or shape different from that of a sintered body of a magnet having a ring shape for forming all of the radial anisotropic magnets and the magnetite particles.

[實施例] [Examples]

以下將本發明之實施例與比較例及參考例對比予以說明。此處所示之實施例、比較例及參考例中使用下述表1之材料。 Hereinafter, embodiments of the present invention will be described in comparison with comparative examples and reference examples. The materials of the following Table 1 were used in the examples, comparative examples and reference examples shown here.

[實施例1] [Example 1]

藉以下順序作成圖4所示形狀之稀土類燒結磁石。 A rare earth sintered magnet having the shape shown in Fig. 4 was produced in the following order.

<粗粉碎> <rough crushing>

對於藉由漏模澆鑄法所得之合金組成(Nd：25.25wt%，Pr：6.75wt%，B：1.01wt%，Ga：0.13wt%，Nb：0.2wt%，Co：2.0wt%，Cu：0.13wt%，Al：0.1wt%，其餘部分Fe，包含其他不可避免雜質)之合金於室溫下吸附氫，以0.85MPa保持1天。隨後，邊以液化Ar冷卻邊以0.2MPa保持1天，而進行氫解碎。 For the alloy composition obtained by the die casting method (Nd: 25.25 wt%, Pr: 6.75 wt%, B: 1.01 wt%, Ga: 0.13 wt%, Nb: 0.2 wt%, Co: 2.0 wt%, Cu: An alloy of 0.13 wt%, Al: 0.1 wt%, and the balance Fe, including other unavoidable impurities, adsorbed hydrogen at room temperature and was kept at 0.85 MPa for 1 day. Subsequently, hydrogen pulverization was carried out while maintaining the liquefied Ar cooling side at 0.2 MPa for 1 day.

<微粉碎> <Micro-crushing>

對於經粗粉碎之合金粗粉100重量份混合己酸甲酯1重量份後，藉由氦噴射研磨機粉碎裝置(裝置名：PJM-80HE，NPK型)進行粉碎。粉碎之合金粒子之捕集係藉由旋風方式分離回收，去除超微粉。粉碎時之供給速度設為1kg/h，He氣體導入壓力為0.6MPa，流量1.3m3/min，氧濃度1ppm以下，露點-75℃以下。藉由微粉碎 所得之磁石材料粒子之平均粒徑為約1.3μm。平均粉碎粒徑係使用雷射繞射/散射式粒徑分佈測定裝置(裝置名：LA950，HORIBA製)進行測定。具體而言，以較低氧化速度使微粉碎粉緩緩氧化後，將數百mg之該緩氧化粉末與矽油(製品名：KF-96H-100萬cs，信越化學製)均一混合作成糊膏狀，將其以石英玻璃夾住作成被試驗樣品(HORIBA糊膏法)。 After 100 parts by weight of the coarsely pulverized alloy coarse powder was mixed with 1 part by weight of methyl hexanoate, the mixture was pulverized by a mash jet mill pulverizing apparatus (device name: PJM-80HE, NPK type). The trapping of the pulverized alloy particles is separated and recovered by a cyclone method to remove the ultrafine powder. The supply speed at the time of pulverization was 1 kg/h, the He gas introduction pressure was 0.6 MPa, the flow rate was 1.3 m 3 /min, the oxygen concentration was 1 ppm or less, and the dew point was -75 ° C or lower. The average particle diameter of the magnet material particles obtained by the fine pulverization was about 1.3 μm. The average pulverized particle diameter was measured using a laser diffraction/scattering type particle size distribution measuring apparatus (device name: LA950, manufactured by HORIBA). Specifically, after the finely pulverized powder is slowly oxidized at a lower oxidation rate, hundreds of mg of the oxidized powder and the eucalyptus oil (product name: KF-96H-100,000 cs, manufactured by Shin-Etsu Chemical Co., Ltd.) are uniformly mixed to form a paste. In the form, it was sandwiched between quartz glass to prepare a test sample (HORIBA paste method).

將粒度分佈(體積%)之圖表中之D50之值設為平均粒徑。惟，粒度分佈為雙峰時，僅對於粒徑小的峰算出D50，作為平均粒徑。 The value of D50 in the graph of the particle size distribution (% by volume) is set as the average particle diameter. However, when the particle size distribution is a double peak, D50 is calculated only for the peak having a small particle diameter as the average particle diameter.

<混練> <mixing>

對於粉碎後之合金粒子100重量份，混合1-辛烯40重量份，藉由混合機(裝置名：TX-0.5，井上製作所製)，於60℃進行加熱攪拌1小時。隨後，減壓蒸餾去除1-辛烯與其反應物進行脫氫處理。於其中添加油醇0.8重量份、1-十八碳烯4.1重量份及聚異丁烯(PIB)B100之甲苯溶液(10重量%)50重量份，於70℃減壓加熱攪拌條件下蒸餾去除甲苯後，進而進行2小時混練，製作黏土狀之複合材料。 For 100 parts by weight of the pulverized alloy particles, 40 parts by weight of 1-octene was mixed, and the mixture was heated and stirred at 60 ° C for 1 hour by a mixer (device name: TX-0.5, manufactured by Inoue Seisakusho Co., Ltd.). Subsequently, 1-octene and its reactants were removed by distillation under reduced pressure for dehydrogenation treatment. Adding 0.8 parts by weight of oleyl alcohol, 4.1 parts by weight of 1-octadecene, and 50 parts by weight of a toluene solution (10% by weight) of polyisobutylene (PIB) B100, and distilling off toluene after heating under stirring at 70 ° C under reduced pressure Further, the mixture was kneaded for 2 hours to prepare a clay-like composite material.

<磁場配向> <Magnetic field alignment>

將該混練步驟作成之複合材料收容於具有與圖10(a)所示形狀相同之空腔之不鏽鋼(SUS)製模具中，形 成第1成形體後，藉由超導電磁線圈(裝置名：JMTD-12T100，JASTEC製)，自外部施加平行磁場而進行配向處理。配向處理係邊施加外部磁場7T邊於80℃進行10分鐘，以對於最短邊方向的梯形厚度方向成為平行之方式施加外部磁場。保持於配向溫度之狀態，自電磁線圈取出，隨後藉由施加逆磁場，實施脫磁處理。逆磁場之施加係使強度自-0.2T至+0.18T，進而至-0.16T變化，邊漸減至零磁場而進行。 The composite material prepared by the kneading step is housed in a mold made of stainless steel (SUS) having the same shape as that shown in Fig. 10(a). After the formation of the first molded body, the alignment treatment was performed by applying a parallel magnetic field from the outside by a superconducting magnetic coil (device name: JMTD-12T100, manufactured by JASTEC). The alignment processing system applied an external magnetic field 7T at 80 ° C for 10 minutes, and applied an external magnetic field so that the trapezoidal thickness direction in the shortest side direction became parallel. The state is maintained at the alignment temperature, taken out from the electromagnetic coil, and then demagnetization treatment is performed by applying a reverse magnetic field. The application of the reverse magnetic field is carried out by changing the intensity from -0.2T to +0.18T, and further to -0.16T, while gradually decreasing to zero magnetic field.

<變形步驟> <deformation step>

配向處理後，自配向處理用之模具取出成形之複合材料之成形加工用薄片，改放入具有比圖10(a)之端部圓弧形狀更淺之端部圓弧形狀之空腔之不鏽鋼(SUS)製之中間成形用模具中，邊於60℃加溫邊加壓。進而取出成形之該成形加工用薄片，改放入具有圖10(b)(c)所示形狀之空腔之不鏽鋼(SUS)製之最終成形用模具中，邊於60℃加溫邊加壓，進行變形。 After the alignment treatment, the formed sheet for forming the composite material is taken out from the mold for processing, and the stainless steel having a cavity having a shallower end arc shape than the end arc shape of the end portion of Fig. 10(a) is placed. The intermediate molding die (SUS) was pressed while being heated at 60 °C. Further, the formed sheet for forming processing was taken out and placed in a final molding die made of stainless steel (SUS) having a cavity having the shape shown in Fig. 10 (b) and (c), and pressed while being heated at 60 °C. , to make deformation.

<鍛燒(脫碳)步驟> <calcining (decarburization) step>

對於變形後之成形加工用薄片，藉0.8Mpa之氫加壓氛圍，進行脫碳處理。以0.8℃/min自室溫升溫至370℃，於該溫度保持3小時。此時之氫流量為2~3L/min。 The deformed sheet for forming processing was subjected to decarburization treatment by a pressurized atmosphere of 0.8 Mpa of hydrogen. The temperature was raised from room temperature to 370 ° C at 0.8 ° C / min, and maintained at this temperature for 3 hours. The hydrogen flow rate at this time is 2 to 3 L/min.

<燒結> <sintering>

脫碳後，於真空中以升溫速度8℃/min升溫至980℃，於該溫度保持2小時而進行燒結。 After decarburization, the temperature was raised to 980 ° C in a vacuum at a rate of temperature increase of 8 ° C / min, and the temperature was maintained at this temperature for 2 hours to carry out sintering.

<燒鈍> <burning>

所得之燒結體，以0.5小時自室溫升溫至500℃後，於500℃保持1小時，隨後急冷而進行燒鈍，獲得稀土類磁石形成用燒結體。 The obtained sintered body was heated from room temperature to 500 ° C in 0.5 hour, and then kept at 500 ° C for 1 hour, and then quenched to be blunt to obtain a sintered body for forming a rare earth magnet.

[實施例2] [Embodiment 2]

除了變更為表2、3所記載之條件以外，進行與實施例1同樣之操作，獲得稀土類磁石形成用燒結體。實施例1與實施例2之梯形磁石厚度不同。 The sintered body for forming a rare earth magnet was obtained in the same manner as in Example 1 except that the conditions described in Tables 2 and 3 were changed. The trapezoidal magnets of Example 1 and Example 2 are different in thickness.

[實施例3] [Example 3]

實施例3中，微粉碎係以球磨機粉碎，於變形後進行脫油步驟，燒結處理設為加壓燒結。實施例3中之球磨機粉碎以後之處理詳述於下。 In Example 3, the fine pulverization was pulverized by a ball mill, and after the deformation, the deoiling step was carried out, and the sintering treatment was carried out under pressure sintering. The treatment after the pulverization of the ball mill in Example 3 is described in detail below.

<粉碎> <Crush>

球磨機粉碎係如下進行。對於氫解碎之合金粗粉100重量份，混合Zr珠粒(2 )1500重量份，投入槽容量0.8L之球磨機(製品名：Attritor 0.8L，日本COKE工業公司製)，以旋轉數500rpm粉碎2小時。添加苯10 重量份作為粉碎時之粉碎助劑，且使用液化Ar作為溶劑。 The ball mill pulverization was carried out as follows. For 100 parts by weight of the hydrogen-crushed alloy coarse powder, mixed Zr beads (2 1500 parts by weight, a ball mill (product name: Attritor 0.8L, manufactured by COKE Corporation, Japan) having a tank capacity of 0.8 L was pulverized at a number of revolutions of 500 rpm for 2 hours. 10 parts by weight of benzene was added as a pulverization aid at the time of pulverization, and liquefied Ar was used as a solvent.

<混練> <mixing>

不進行1-辛烯之脫氫，而混合作為配向潤滑劑之1-十八碳炔6.7重量份及作為聚合物之聚異丁烯(PIB)(製品名：B150，BASF公司製)之甲苯溶液(8重量%)50重量份，藉由混合機(裝置名：TX-0.5，井上製作所製)，於70℃進行減壓加熱攪拌。餾除甲苯後，進而減壓下進行2小時混練，製作黏土狀之複合材料。 Without dehydrogenation of 1-octene, 6.7 parts by weight of 1-octadecene alkyne as a matching lubricant and a toluene solution of polyisobutylene (PIB) (product name: B150, manufactured by BASF Corporation) as a polymer ( 8% by weight of 50 parts by weight, and the mixture was heated under reduced pressure at 70 ° C by a mixer (device name: TX-0.5, manufactured by Inoue Seisakusho Co., Ltd.). After toluene was distilled off, the mixture was further kneaded under reduced pressure for 2 hours to prepare a clay-like composite material.

<磁場配向> <Magnetic field alignment>

將複合材料填充於具有與圖10(a)之形狀相同之空腔之SUS製模具後，藉由超導電磁線圈(裝置名：JMTD-12T100，JASTEC製)，進行配向處理。配向處理係於外部磁場7T、80℃進行10分鐘，以對於最短邊方向(梯形厚度方向)成為平行之方式施加外部磁場。保持於配向溫度之狀態，自電磁線圈取出，隨後藉由施加逆磁場，實施脫磁處理。逆磁場之施加係使強度自-0.2T至+0.18T，進而至-0.16T變化，邊漸減至零磁場而進行。 After the composite material was filled in a SUS mold having a cavity having the same shape as that of FIG. 10(a), the alignment treatment was performed by a superconducting magnetic coil (device name: JMTD-12T100, manufactured by JASTEC). The alignment treatment was performed for 10 minutes at an external magnetic field 7T and 80 ° C, and an external magnetic field was applied so that the shortest side direction (trapezoidal thickness direction) was parallel. The state is maintained at the alignment temperature, taken out from the electromagnetic coil, and then demagnetization treatment is performed by applying a reverse magnetic field. The application of the reverse magnetic field is carried out by changing the intensity from -0.2T to +0.18T, and further to -0.16T, while gradually decreasing to zero magnetic field.

<變形步驟> <deformation step>

配向處理後，自配向處理用之模具取出成形之複合材料之成形加工用薄片，改放入具有比圖10(a)之 端部圓弧形狀更淺之端部圓弧形狀之空腔之不鏽鋼(SUS)製之中間成形用模具中，邊於60℃加溫邊加壓。進而取出成形之該成形加工用薄片，改放入具有圖10(b)(c)所示形狀之空腔之不鏽鋼(SUS)製之最終成形用模具中，邊於60℃加溫邊加壓，進行變形。變形後，自SUS模具取出複合材料，***具有與圖10(b)相同形狀之空腔之石墨模具中。石墨模具之空腔具有長度方向長度比成形之梯型形狀複合材料之長度方向長20mm左右之空腔，以位於空腔之中央部之方式***。於石墨模具中預先塗佈BN(氮化硼)粉末作為脫模材。 After the alignment treatment, the formed sheet for forming the composite material is taken out from the mold for processing, and is placed in a sheet having a higher ratio than that of FIG. 10(a). In the intermediate molding die made of stainless steel (SUS) having a shallower end arc shape and a cavity having an arc shape at the end, it is pressurized while being heated at 60 °C. Further, the formed sheet for forming processing was taken out and placed in a final molding die made of stainless steel (SUS) having a cavity having the shape shown in Fig. 10 (b) and (c), and pressed while being heated at 60 °C. , to make deformation. After the deformation, the composite material was taken out from the SUS mold, and inserted into a graphite mold having a cavity having the same shape as that of Fig. 10(b). The cavity of the graphite mold has a cavity whose length in the longitudinal direction is longer than the longitudinal direction of the formed ladder-shaped composite material, and is inserted so as to be located at the central portion of the cavity. BN (boron nitride) powder was previously applied as a release material in a graphite mold.

<脫油步驟> <Deoiling step>

對於***石墨模具中之複合材料，在減壓氛圍下，進行脫油處理。排氣泵係以旋轉泵進行，以0.9℃/min自室溫升溫至100℃，保持60小時。藉由該步驟，如配向潤滑劑、可塑劑之油成分可藉由揮發而去除。 For the composite material inserted into the graphite mold, deoiling treatment is carried out under a reduced pressure atmosphere. The exhaust pump was operated by a rotary pump and heated from room temperature to 100 ° C at 0.9 ° C / min for 60 hours. By this step, the oil component such as the alignment lubricant and the plasticizer can be removed by volatilization.

<鍛燒(脫碳)步驟> <calcining (decarburization) step>

對於進行脫油處理之複合材料，於0.8MPa之氫加壓氛圍下進行脫碳處理。以2.9℃/min自室溫升溫至370℃，保持2小時。且氫流量對於約1L之加壓容器為2~3L/min。 The decarburization treatment was carried out on a composite material subjected to deoiling treatment under a hydrogen pressure atmosphere of 0.8 MPa. The temperature was raised from room temperature to 370 ° C at 2.9 ° C / min for 2 hours. And the hydrogen flow rate is 2 to 3 L/min for a pressurized container of about 1 L.

<燒結> <sintering>

脫碳後，將具有與圖10(b)相同形狀之石墨製按壓銷***石墨模具中，藉由加壓按壓銷，於減壓氛圍下進行加壓燒結。以加壓方向為對於c軸配向方向垂直方向(平行於樣品長度方向)進行。燒結係邊施加0.37MPa之加壓作為初期荷重，邊以19.3℃/min升溫至700℃。隨後，於9.2MPa加壓下以7.1℃/min升溫至最終燒結溫度的950℃，於950℃保持5分鐘而進行。 After decarburization, a graphite press pin having the same shape as that of Fig. 10 (b) was inserted into a graphite mold, and pressure-sintering was performed under a reduced pressure atmosphere by pressurizing the press pin. The pressing direction is performed in the vertical direction (parallel to the sample length direction) with respect to the c-axis alignment direction. A pressurization of 0.37 MPa was applied to the sintering system as an initial load, and the temperature was raised to 700 ° C at 19.3 ° C / min. Subsequently, the temperature was raised to 950 ° C at a final sintering temperature of 7.1 ° C / min under a pressure of 9.2 MPa, and the temperature was maintained at 950 ° C for 5 minutes.

<燒結粒徑> <Sintered particle size>

所得燒結體之燒結粒徑係藉由利用SiC紙研磨，利用拋光研磨及利用銑床對燒結體表面實施表面處理後，藉由具備EBSD檢測器(裝置名：AZtecHKL EBSD NordlysNano Integrated,Oxford Instruments製)之SEM(裝 置名：JSM-7001F，日本電子製)或具備EDAX公司製之EBSD檢測器(Hikari High Speed EBSD Detector)之掃描電子顯微鏡(ZEISS公司製SUPRA40VP)分析。視角係設定為粒子個數至少進入200個以上，步階設為0.1~1μm。 The sintered particle size of the obtained sintered body was polished by SiC paper, and the surface of the sintered body was subjected to surface treatment by buffing and milling using a EBSD detector (device name: AZtecHKL EBSD Nordlys Nano Integrated, manufactured by Oxford Instruments). SEM The name is JSM-7001F (manufactured by JEOL Ltd.) or a scanning electron microscope (SUPRA40VP manufactured by ZEISS Co., Ltd.) equipped with an EBSD detector (Hikari High Speed EBSD Detector) manufactured by EDAX. The viewing angle is set such that the number of particles enters at least 200 or more, and the step is set to 0.1 to 1 μm.

分析數據利用Chanel5(Oxford Instruments製)或OIM解析軟體ver5.2(EDAX公司製)進行解析，粒界之判斷係將結晶方位之偏移角度成為2°以上之部分作為粒界層，進行處理。僅抽出主相，將其相當圓之直徑之個數平均值設為燒結粒徑。 The analysis data was analyzed by using Chanel 5 (manufactured by Oxford Instruments) or OIM analysis software ver5.2 (manufactured by EDAX Co., Ltd.), and the grain boundary was judged by treating the portion having an offset angle of crystal orientation of 2 or more as a grain boundary layer. Only the main phase is taken out, and the average of the number of the diameters of the equivalent circles is set as the sintered particle diameter.

<配向角偏差角度△θ之半值寬之測定> <Measurement of Half Value Width of Alignment Angle Deviation Angle Δθ>

所得之燒結體之配向角度，係對於燒結體表面利用SiC紙研磨、拋光研磨、銑床實施表面處理後，藉由具備EBSD檢測器(裝置名：AZtecHKL EBSD NordlysNano Integrated,Oxford Instruments製)之SEM(裝置名：JSM-7001F，日本電子製)或具備EDAX公司製之EBSD檢測器(Hikari High Speed EBSD Detector)之掃描電子顯微鏡(ZEISS公司製SUPRA40VP)分析。又，EBSD之分析係以35μm之視角以0.2μm間距進行。為了提高分析精度，對於進入有至少30個燒結粒子之方式進行分析。 The alignment angle of the obtained sintered body is SEM (apparatus: AZtecHKL EBSD Nordlys Nano Integrated, manufactured by Oxford Instruments) equipped with an EBSD detector (surface name: AZtecHKL EBSD Nordlys Nano Integrated, manufactured by Oxford Instruments) after the surface of the sintered body is polished by SiC paper, polished, and milled. Name: JSM-7001F, manufactured by JEOL Ltd. or a scanning electron microscope (SUPRA40VP manufactured by ZEISS) equipped with an EDAX EBSD detector (Hikari High Speed EBSD Detector). Further, the analysis of EBSD was carried out at a pitch of 0.2 μm from a viewing angle of 35 μm. In order to improve the analysis accuracy, the analysis was carried out in such a manner that at least 30 sintered particles were entered.

本實施例中，將燒結體的梯形磁石於寬度方向中央切斷，於其剖面進行測定。測定係於該剖面之厚度方向中央，於梯形左端附近及右端附近與中央附近合計3處進行分析。 In the present embodiment, the trapezoidal magnet of the sintered body was cut at the center in the width direction, and the cross section was measured. The measurement was performed at the center in the thickness direction of the cross section, and three points were analyzed in the vicinity of the left end of the trapezoid and the vicinity of the right end and the vicinity of the center.

於各分析位置，將易磁化軸頻度最高朝向之方向設為該分析位置之配向軸方向，將配向軸方向相對於基準面之角度設為配向軸角度，如圖3(a)所示，梯形底面成為包含A2軸與A3軸之平面時，以該平面為基準面，求出自A1軸朝A3軸方向之配向軸之傾斜角α與自A1軸朝A2軸方向之配向軸之傾斜角(θ+β)作為配向軸角度。於包含A1軸及A2軸之平面，任一分析位置係易磁化軸之特定配向方向均位於包含該A1軸及A2軸之平面內。因此，傾斜角α成為自易磁化軸之特定配向方向之位移量亦即「偏移角」。且與角β關連使用之角θ於任意分析位置中係所設計之易磁化軸配向方向與A1軸之間之角度，因此，角β係相對於該分析位置之配向軸之特定配向方向之位移量亦即「偏移角」。 At each analysis position, the direction of the highest axis of the easy magnetization axis is the direction of the alignment axis of the analysis position, and the angle of the alignment axis direction with respect to the reference plane is the alignment axis angle, as shown in Fig. 3(a), trapezoidal When the bottom surface is a plane including the A2 axis and the A3 axis, the inclination angle α of the alignment axis from the A1 axis toward the A3 axis direction and the inclination angle of the alignment axis from the A1 axis direction to the A2 axis direction are obtained using the plane as a reference plane ( θ+β) is the angle of the alignment axis. In the plane including the A1 axis and the A2 axis, the specific alignment direction of any of the analysis positions of the easy magnetization axis is in the plane including the A1 axis and the A2 axis. Therefore, the inclination angle α becomes the "offset angle" which is the displacement amount from the specific alignment direction of the easy magnetization axis. And the angle θ used in relation to the angle β is an angle between the alignment direction of the easy magnetization axis and the A1 axis designed in any analysis position, and therefore, the displacement of the angle β relative to the specific alignment direction of the alignment axis of the analysis position The quantity is also the "offset angle".

針對各分析位置中角度差最大之2個配向向量(本實施例中，為梯形左端附近/右端附近之配向向量)，求出該等配向向量嵌之角度，算出配向軸角度差(0°≦≦90°)。 For the two alignment vectors with the largest angular difference among the analysis positions (in the present embodiment, the alignment vector near the left end of the trapezoid or near the right end), the angles of the alignment vectors are obtained, and the angle difference of the alignment axes is calculated. (0°≦ ≦90°).

且，各分析位置之EBSD分析時，將配向向量之方向修正為0°後，以測定粒子單位算出相對於0°方向之磁石材料粒子之易磁化軸的結晶C軸(001)之偏移角度，將該偏移角度之頻度自90°至0°累積之累積比率作圖為圖表，求出累計比率為50%之角度作為「配向角偏差角度△θ之半值寬」。 Further, in the EBSD analysis of each analysis position, after the direction of the alignment vector is corrected to 0°, the offset angle of the crystal C-axis (001) with respect to the easy magnetization axis of the magnet material particles in the 0° direction is calculated in units of measured particles. The cumulative ratio of the frequency of the offset angle from 90° to 0° is plotted as a graph, and the angle at which the cumulative ratio is 50% is obtained as the "half-value width of the alignment angle deviation angle Δθ".

<燒結粒子之長寬比> <Aspect of the aspect ratio of sintered particles>

所得之燒結體之燒結粒子之長寬比，係對於燒結體表面利用SiC紙研磨、拋光研磨、銑床之一或兩者以上組合實施表面處理後，藉由具備EBSD檢測器(裝置名：AZtecHKL EBSD NordlysNano Integrated,Oxford Instruments製)之SEM(裝置名：JSM-7001F，日本電子製)分析。視角係設定為粒子個數至少進入有100個以上，步階設為0.1~1μm。 The aspect ratio of the sintered particles of the obtained sintered body is obtained by subjecting the surface of the sintered body to surface treatment by SiC paper polishing, buffing, milling, or a combination of two or more, and then having an EBSD detector (device name: AZtecHKL EBSD) SEM (device name: JSM-7001F, manufactured by Nippon Electronics Co., Ltd.) of Nordlys Nano Integrated, manufactured by Oxford Instruments. The viewing angle is set such that the number of particles enters at least 100 or more, and the step is set to 0.1 to 1 μm.

分析數據利用Chanel5(Oxford Instruments製)進行解析，粒界之判斷係將結晶方位之偏移角度成為2°以上之部分作為粒界層，進行處理，獲得粒界抽出像。對於所得粒界抽出像，利用ImageJ(Wayne Rasband製)，算出與粒子形狀外切之長方形中最長邊之長度(a)與最短邊長度(b)，將其比之平均值設為長寬比(a/b)。 The analysis data was analyzed by Chanel 5 (manufactured by Oxford Instruments), and the grain boundary was determined by using a portion having an offset angle of crystal orientation of 2 or more as a grain boundary layer to obtain a grain boundary extraction image. With respect to the obtained grain boundary extraction image, the length (a) and the shortest side length (b) of the longest side of the rectangle excised from the particle shape were calculated by ImageJ (manufactured by Wayne Rasband), and the average value was set to the aspect ratio. (a/b).

所得實施例1~3之評價結果示於表4。 The evaluation results of the obtained Examples 1 to 3 are shown in Table 4.

實施例1~實施例3之任一者，均如所期待，可知藉由複合材料之彎曲加工，配向向量朝向梯形中心方向集中。且，個分析位置之配向向量所成之角係至少 20°以上，確認並非平行配向。再者，個分析位置之配向角偏差角度之指標的△θ之半值寬之值為10°~16°左右，可確認為非平行磁石並且為偏差小的磁石。 As in any of the first to third embodiments, as expected, it was found that the alignment vector was concentrated toward the trapezoidal center direction by the bending of the composite material. And the angle of the alignment vector of the analysis position It is at least 20° or more, and it is confirmed that it is not parallel alignment. In addition, the value of the half value width of Δθ of the index of the deviation angle of the analysis position is about 10° to 16°, and it can be confirmed that it is a non-parallel magnet and is a magnet having a small deviation.

[實施例4] [Example 4]

<粗粉碎> <rough crushing>

藉由漏模澆鑄法所得之與實施例1同樣之合金組成之合金在室溫下吸附氫，於0.85MPa保持1天。隨後，邊冷卻藉由於0.2MPa保持1天進行氫解碎。 The alloy having the same alloy composition as that of Example 1 obtained by the die casting method was adsorbed with hydrogen at room temperature and kept at 0.85 MPa for 1 day. Subsequently, the side cooling was carried out by hydrogen disintegration by keeping it at 0.2 MPa for 1 day.

<微粉碎> <Micro-crushing>

對於氫粉碎之合金粗粉100重量份混合己酸甲酯1重量份後，藉由氦噴射研磨機粉碎裝置(裝置名：PJM-80HE，NPK型)進行粉碎。粉碎之合金粒子之捕集係藉由旋風方式分離回收，去除超微粉。粉碎時之供給速度設為1kg/h，He氣體導入壓力為0.6MPa，流量為1.3m3/min，氧濃度為1ppm以下，露點為-75℃以下。所得粉碎粉之平均粒徑為約1.2μm。平均粉碎粒徑係藉由與實施例1同樣方法測定。 After 100 parts by weight of the hydrogen pulverized alloy coarse powder was mixed with 1 part by weight of methyl hexanoate, the mixture was pulverized by a mash jet mill pulverizing apparatus (device name: PJM-80HE, NPK type). The trapping of the pulverized alloy particles is separated and recovered by a cyclone method to remove the ultrafine powder. The supply speed at the time of pulverization was 1 kg/h, the He gas introduction pressure was 0.6 MPa, the flow rate was 1.3 m 3 /min, the oxygen concentration was 1 ppm or less, and the dew point was -75 ° C or lower. The obtained pulverized powder had an average particle diameter of about 1.2 μm. The average pulverized particle diameter was measured in the same manner as in Example 1.

<混練> <mixing>

對於粉碎後之合金粒子100重量份，混合1-辛烯40重量份，藉由混合機(裝置名：TX-5，井上製作所製)，於60℃進行加熱攪拌1小時。隨後，藉由減壓加熱 蒸餾去除1-辛烯與其反應物進行脫氫處理。其次，對於合金粒子，添加1-十八碳炔1.7重量份、1-十八碳烯4.3重量份及聚異丁烯(PIB：BASF公司製，oppanol B150)之甲苯溶液(8重量%)50重量份，邊於70℃加熱攪拌邊減壓而蒸餾去除甲苯。隨後，進而減壓下邊於70℃加熱進行2小時混練，製作黏土狀之複合材料。 For 100 parts by weight of the pulverized alloy particles, 40 parts by weight of 1-octene was mixed, and the mixture was heated and stirred at 60 ° C for 1 hour by a mixer (device name: TX-5, manufactured by Inoue Seisakusho Co., Ltd.). Subsequently, heated by decompression The 1-octene and its reactants are distilled off to carry out dehydrogenation treatment. Next, 1.7 parts by weight of 1-octadecyne, 4.3 parts by weight of 1-octadecene, and 50 parts by weight of a toluene solution (8 wt%) of polyisobutylene (PIB: manufactured by BASF Corporation, oppanol B150) were added to the alloy particles. The toluene was distilled off under reduced pressure while heating and stirring at 70 °C. Subsequently, the mixture was further heated under reduced pressure at 70 ° C for 2 hours to prepare a clay-like composite material.

<第1成形體之形成> <Formation of the first molded body>

將上述混練步驟作成之複合材料收容於具有與圖16所示形狀相同之空腔之不鏽鋼(SUS)製模具中，形成平板形狀之第1成形體。 The composite material prepared by the kneading step was housed in a stainless steel (SUS) mold having a cavity having the same shape as that shown in Fig. 16, and a first molded body having a flat plate shape was formed.

<磁場配向> <Magnetic field alignment>

對收容有複合材料之不鏽鋼(SUS)製模具，藉由超導電磁線圈(裝置名：JMTD-7T200，JASTEC製)，於圖16所示方向自外部施加平行磁場而進行配向處理。該配向係將收容有複合材料之不鏽鋼(SUS)製之模具加熱至80℃，將外部磁場設為7T之狀態，以10分鐘時間通過具有2000mm之軸長之超導電磁線圈之內部而進行。隨後使用脈衝式脫磁裝置(MFC-2506D，MAGNET FORCE公司製)，對收容有複合材料之不鏽鋼(SUS)製之模具施加脈衝磁場，進行複合材料之脫磁。 A stainless steel (SUS) mold containing a composite material was subjected to an alignment treatment by applying a parallel magnetic field from the outside in a direction shown in FIG. 16 by a superconducting magnetic coil (device name: JMTD-7T200, manufactured by JASTEC). In the alignment, the mold made of stainless steel (SUS) containing the composite material was heated to 80 ° C, and the external magnetic field was set to 7 T, and the inside of the superconducting magnetic coil having an axial length of 2000 mm was passed for 10 minutes. Subsequently, a pulsed magnetic field was applied to a mold made of stainless steel (SUS) containing a composite material using a pulse demagnetization device (MFC-2506D, manufactured by MAGNET FORCE Co., Ltd.) to demagnetize the composite material.

<第2成形體之形成> <Formation of second molded body>

將如上述進行脫磁處理之第1成形體自不鏽鋼製之模具取出，收容於具有曲率半徑為48.75mm之圓弧狀空腔之母模中，藉由以具有曲率半徑為45.25mm的圓弧狀模面之公模按壓，使該第1成形體變形，形成第1中間成形體(圖17(a))。其次，將第1該中間成形體收容於具有曲率半徑為25.25mm之圓弧狀空腔之母模中，藉由以具有曲率半徑為21.75mm的圓弧狀模面之公模按壓，使該第1中間成形體變形，形成第2中間成形體(圖17(b))。進而，將該第2中間成形體收容於具有曲率半徑為17.42mm之圓弧狀空腔之母模中，藉由以具有曲率半徑為13.92mm的圓弧狀模面之公模按壓，使該第2中間成形體變形，形成第3中間成形體(圖17(c))。隨後，將該第3中間成形體收容於具有曲率半徑為13.50mm之圓弧狀空腔之母模中，藉由以具有曲率半徑為10.00mm的圓弧狀模面之公模按壓，使該第3中間成形體變形，形成具有半圓形之圓弧形狀剖面之第2成形體(圖17(d))。朝中間成形體及第2成形體之變形均在70℃之溫度條件進行，控制為變形後之厚度無變化。 The first molded body subjected to the demagnetization treatment as described above was taken out from a mold made of stainless steel, and housed in a mother mold having an arc-shaped cavity having a radius of curvature of 48.75 mm, by having an arc having a radius of curvature of 45.25 mm. The male mold of the mold surface is pressed to deform the first molded body to form a first intermediate formed body (Fig. 17 (a)). Next, the first intermediate formed body is housed in a master mold having an arcuate cavity having a radius of curvature of 25.25 mm, and is pressed by a male mold having an arcuate mold surface having a curvature radius of 21.75 mm. The first intermediate formed body is deformed to form a second intermediate formed body (Fig. 17(b)). Further, the second intermediate formed body is housed in a master mold having an arcuate cavity having a radius of curvature of 17.42 mm, and is pressed by a male mold having an arcuate mold surface having a curvature radius of 13.92 mm. The second intermediate formed body is deformed to form a third intermediate formed body (Fig. 17 (c)). Subsequently, the third intermediate formed body is housed in a master mold having an arcuate cavity having a radius of curvature of 13.50 mm, and is pressed by a male mold having an arcuate mold surface having a radius of curvature of 10.00 mm. The third intermediate formed body is deformed to form a second molded body having a semicircular arc-shaped cross section (Fig. 17 (d)). The deformation of the intermediate formed body and the second molded body was carried out at a temperature of 70 ° C, and the thickness after the deformation was controlled to be unchanged.

<鍛燒(脫碳)> <calcining (decarburization)>

對於第2成形體，於0.8MPa之高壓氫氣之脫碳爐中，以下述之溫度條件進行脫碳處理。脫碳處理係藉由以1.0℃/min自室溫升溫至500℃，於500℃之溫度保持2小時而進行，該處理過程中，藉由吹入氫氣，以使有機 物之分解物不滯留於脫碳爐中。氫流量為2L/min。 The second molded body was subjected to a decarburization treatment under the following temperature conditions in a decarburization furnace of high pressure hydrogen gas of 0.8 MPa. The decarburization treatment is carried out by raising the temperature from room temperature to 500 ° C at 1.0 ° C / min and maintaining at a temperature of 500 ° C for 2 hours. During the treatment, hydrogen is blown to make the organic The decomposition product does not remain in the decarburization furnace. The hydrogen flow rate was 2 L/min.

<燒結> <sintering>

脫碳後之成形體於減壓氛圍中燒結。燒結係藉由以2小時升溫至970℃(升溫速度7.9℃/min)，於970℃之溫度保持2小時而進行。所得燒結體於燒結後冷卻至室溫。 The shaped body after decarburization is sintered in a reduced pressure atmosphere. The sintering was carried out by raising the temperature to 970 ° C for 2 hours (heating rate 7.9 ° C / min) and maintaining the temperature at 970 ° C for 2 hours. The obtained sintered body was cooled to room temperature after sintering.

<燒鈍> <burning>

所得之燒結體，以0.5小時自室溫升溫至500℃後，於500℃之溫度保持1小時，隨後急冷而進行燒鈍，獲得圖18所示之具有半圓形之圓弧狀剖面之稀土類磁石形成用燒結體。 The obtained sintered body was heated from room temperature to 500 ° C in 0.5 hour, and then kept at a temperature of 500 ° C for 1 hour, followed by rapid cooling to be blunt, and a rare earth having a semicircular arc-shaped cross section as shown in FIG. 18 was obtained. A sintered body for forming a magnet.

<配向軸角度、配向角偏差角度之測定> <Measurement of the angle of the alignment axis and the angle of deviation of the alignment angle>

針對所得燒結體以與實施例1同樣方法進行測定。惟，本實施例中，將具有圓弧形狀剖面及與該圓弧形狀剖面正交之長度方向之燒結體於長度方向中央於橫剖面方向切斷，於該剖面進行測定。圖18中顯示供於分析之具有半圓形之圓弧形狀剖面之稀土類磁石形成用燒結體之剖面。該燒結體具有以將兩端部間連結之直徑線表示之直徑方向D、圓弧之曲率中心O、沿著徑向之該燒結體厚度T、及周方向S。與圖18之紙面直角之方向為長度方向L。 The obtained sintered body was measured in the same manner as in Example 1. In the present embodiment, the sintered body having a circular arc-shaped cross section and a longitudinal direction orthogonal to the circular arc-shaped cross-section is cut in the longitudinal direction at the center in the longitudinal direction, and is measured in the cross section. Fig. 18 is a cross section showing a sintered body for forming a rare earth magnet having a semicircular arc-shaped cross section for analysis. The sintered body has a diameter direction D indicated by a diameter line connecting the both end portions, a curvature center O of the circular arc, a thickness T of the sintered body along the radial direction, and a circumferential direction S. The direction perpendicular to the plane of the paper of Fig. 18 is the longitudinal direction L.

用以獲得配向軸角度及配向角偏差角度之測定場所，係將沿著該圓弧形狀剖面之半徑方向通過厚度T之厚度中心之厚度中心圓弧分為4等份之點所決定之3點，亦即厚度中心圓弧之周方向中心點與燒結體左端之厚度中心間之中點(圖18分析位置a)、厚度中心圓弧之周方向中心點(圖18分析位置b)、厚度中心圓弧之周方向中心點與燒結體右端之厚度中心間之中點(圖18分析位置c3)。又，於沿著包含圖18之分析位置c3之半徑方向線之部位，對距圓弧凸側表面300μm之靠近半徑方向內側之點(圖18分析位置c1)、該凸側表面與厚度中心之點(c3)之間之中點(圖18分析位置c2)、圓弧之凹側表面與厚度中心之點(c3)之間之中點(圖18分析位置c4)、距凹側表面300μm之靠近半徑方向外側之點(圖18分析位置c5)之5點進行測定。 The measurement site for obtaining the angle of the alignment axis and the deviation angle of the alignment angle is determined by dividing the radius center of the thickness of the circular arc shape into three points determined by dividing the center circular arc of the thickness center of the thickness T into four equal parts. That is, the midpoint between the center point of the circumferential center of the thickness center arc and the center of the thickness of the left end of the sintered body (analysis position a in Fig. 18), the center point in the circumferential direction of the center arc of the thickness (analysis position b in Fig. 18), and the center of thickness The midpoint between the center point of the arc in the circumferential direction and the center of the thickness of the right end of the sintered body (analysis position c3 in Fig. 18). Further, at a portion along the radial direction line including the analysis position c3 of Fig. 18, a point closer to the inner side in the radial direction from the convex side surface of the circular arc (the analysis position c1 in Fig. 18), the convex side surface and the thickness center The midpoint between the points (c3) (analysis position c2 in Fig. 18), the midpoint between the concave side surface of the circular arc and the point (c3) of the thickness center (analysis position c4 in Fig. 18), 300 μm from the concave side surface The measurement was performed at 5 points near the point on the outer side in the radial direction (analysis position c5 in Fig. 18).

稀土類磁石形成用燒結體之上述分析位置之各者中，磁石材料粒子之易磁化軸亦即該磁石材料粒子之結晶C軸(001)以最高頻度朝向之方向設為該分析位置之配向軸方向。如圖19所示，設定於燒結體之包含半圓形圓弧形狀剖面之平面內，自曲率中心O通過燒結體之厚度中心圓弧之周方向中心點(圖18分析位置b)之半徑線設為A1軸，同平面內之通過該曲率中心O之與該A1軸正交之半徑線設為A2軸，通過該曲率中心O且與該A1軸及A2軸兩者正交之於燒結體長度方向延伸之線設為A3軸之正交座標系，包含該A2軸與A3軸之平面定為基準面。 因此，求出自A1軸朝向A3軸方向之易磁化軸之配向方向之傾斜角α、與自A1軸朝向A2軸方向之易磁化軸之傾斜角(θ+β)。於包含A1軸及A2軸之平面，於任一分析位置，易磁化軸之特定配向方向位於包含該A1軸及A2軸之平面內。因此，傾斜角α成為易磁化軸自特定之設計上之配向方向之位移量，亦即「偏移角」。且，與角β關連使用之角θ係連結任意分析位置與曲率中心O之半徑線與A1軸之間之角度，因此，角β係相對於該分析位置之配向軸之特定配向方向之位移量亦即「偏移角」。 In each of the analysis positions of the sintered body for forming a rare earth magnet, the axis of easy magnetization of the magnet material particles, that is, the crystal C-axis (001) of the magnet material particles is oriented at the highest frequency toward the alignment axis of the analysis position. direction. As shown in Fig. 19, in the plane of the sintered body including the semicircular arc-shaped cross section, the radius from the center of curvature O through the center point of the circumferential center arc of the thickness of the sintered body (analysis position b in Fig. 18) The axis is the A1 axis, and the radius line orthogonal to the A1 axis passing through the center of curvature O in the same plane is set to the A2 axis, and the curvature center O is orthogonal to the A1 axis and the A2 axis to the sintered body. The line extending in the longitudinal direction is set as the orthogonal coordinate system of the A3 axis, and the plane including the A2 axis and the A3 axis is defined as the reference plane. Therefore, the inclination angle α of the alignment direction of the easy magnetization axis from the A1 axis toward the A3 axis direction and the inclination angle (θ+β) of the easy magnetization axis from the A1 axis toward the A2 axis direction are obtained. In a plane including the A1 axis and the A2 axis, at any analysis position, the specific alignment direction of the easy magnetization axis lies in a plane including the A1 axis and the A2 axis. Therefore, the inclination angle α becomes the displacement amount of the easy magnetization axis from the specific alignment direction of the design, that is, the "offset angle". Moreover, the angle θ used in connection with the angle β connects the angle between the arbitrary analysis position and the radius line of the curvature center O and the A1 axis, and therefore, the displacement of the angle β relative to the specific alignment direction of the alignment axis of the analysis position. That is, the "offset angle".

針對各分析位置，針對特定數以上之磁石材料粒子之易磁化軸進行配向軸分析。作為磁石材料粒子之特定數，較好以分析位置中包含至少30個磁石材料粒子之方式決定分析位置範圍。本實施例中，以針對約700個磁石材料粒子進行測定之方式，決定分析位置之範圍。 For each analysis position, the alignment axis analysis is performed for the easy magnetization axis of a specific number or more of the magnet material particles. As the specific number of the magnet material particles, it is preferred to determine the analysis position range such that at least 30 magnet material particles are included in the analysis position. In the present embodiment, the range of the analysis position is determined in such a manner as to measure about 700 magnet material particles.

且，於各分析位置之EBSD分析時，將各分析位置之基準配向軸方向修正為0°後，對每個磁石材料粒子算出對於基準配向軸方向的0°方向之各磁石材料粒子之易磁化軸之配向軸方向作為角度差△θ，將該角度差△θ之頻度自90°至0°累積之累積比率作圖為圖表，求出累計比率為50%之角度作為配向角偏差角度(△θ之半值寬)。再者，求出各分析位置之最大配向軸角度之差的配向軸角度差。分析結果示於表5。 Further, in the EBSD analysis of each analysis position, after the reference alignment axis direction of each analysis position is corrected to 0°, the magnetization of each magnet material particle in the 0° direction with respect to the reference alignment axis direction is calculated for each magnet material particle. The direction of the axis of the axis is the angle difference Δθ, and the cumulative ratio of the frequency of the angle difference Δθ from 90° to 0° is plotted as a graph, and the angle at which the cumulative ratio is 50% is obtained as the angle of deviation of the alignment angle (Δ). Half value of θ is wide). Furthermore, the angle difference of the alignment axis of the difference between the maximum alignment axis angles of the respective analysis positions is obtained. . The results of the analysis are shown in Table 5.

測定部位之角β值為4°以下，可確認可製作如設計之徑向配向之燒結體。且，△θ之半值寬之最大為11.1°，亦確認為配向角偏差角度小的燒結體。又，配向軸角度差為89°，可確認成為非平行配向。 The angle β of the measurement site was 4° or less, and it was confirmed that a sintered body having a radial alignment as designed can be produced. Further, the maximum value of the half value width of Δθ was 11.1°, and it was confirmed that the sintered body had a small angle of deviation of the alignment angle. Also, the angle difference of the alignment axis At 89°, it was confirmed that it became a non-parallel alignment.

[實施例5~9] [Examples 5 to 9]

除了變更如表6所示之第2成形體之形成中之曲角度以及第1成形體、中間成形體1~3及第2成形體之尺寸以外，進行與實施例4同樣操作，獲得實施例5~9之燒結體。 The same procedure as in Example 4 was carried out except that the bending angle in the formation of the second molded body shown in Table 6 and the dimensions of the first molded body, the intermediate molded bodies 1 to 3, and the second molded body were changed. 5~9 sintered body.

又，成形係於每各成形階段產生45°變形之方式進行。例如於實施例5中，藉由對由圖16所示之模具成形之第1成形體進行如圖17(a)所示之45°變形而成為中間成形體1，如圖17(b)所示，進而進行45°之變形，製造賦予合計90°變形之第2成形體。實施例7中，進而賦予45°變形而形成如圖17(c)所示之第2成形體。實施例6、8、9中，進而賦予45°變形而形成如圖17(d)所示之第2成形體。惟，實施例9中，於配向步驟中藉由超導電磁線圈 (裝置名：JMTD-12T100，JASTEC製)，自外部施加平行磁場而進行配向處理。該配向處理係將收容有複合材料之不鏽鋼(SUS)製模具邊加溫至80℃邊設置於超導電磁線圈內，以20分鐘自0T升磁至7T，隨後，以20分鐘減磁至0T而實施。進而隨後，藉由施加逆磁場實施脫磁處理。逆磁場之施加係使強度自-0.2T至+0.18T，進而至-0.16T變化，邊漸減至零磁場而進行。 Further, the molding was carried out in such a manner that 45° deformation occurred in each molding stage. For example, in the fifth embodiment, the first molded body formed by the mold shown in Fig. 16 is deformed by 45° as shown in Fig. 17(a) to form the intermediate formed body 1, as shown in Fig. 17(b). Further, deformation was performed at 45° to produce a second molded body which was deformed by a total of 90°. In the seventh embodiment, a 45° deformation was further imparted to form a second molded body as shown in Fig. 17(c). In Examples 6, 8, and 9, a second molded body as shown in Fig. 17 (d) was formed by further deforming at 45°. However, in the embodiment 9, the superconducting magnetic coil is used in the alignment step. (Device name: JMTD-12T100, manufactured by JASTEC), and a parallel magnetic field was applied from the outside to perform alignment processing. In the alignment treatment, a stainless steel (SUS) mold containing a composite material was placed in a superconducting magnetic coil while being heated to 80 ° C, and magnetized from 0 T to 7 T in 20 minutes, and then demagnetized to 0 T in 20 minutes. And implementation. Further, demagnetization treatment is then carried out by applying a reverse magnetic field. The application of the reverse magnetic field is carried out by changing the intensity from -0.2T to +0.18T, and further to -0.16T, while gradually decreasing to zero magnetic field.

各燒結體之評價結果示於表7及表8。 The evaluation results of the respective sintered bodies are shown in Tables 7 and 8.

實施例5~9中，於測定部位之角β最大為9°，可知藉由變形操作獲得顯示如設計之徑向配向之燒結體。且，可確認任一實施例之情況，最大配向軸角度差均為20°以上之非平行配向。實施例9之配向角偏差雖稍大，但此認為係因為配向裝置之差所致者。若使用與實施例4~8同樣裝置，則認為實施例9之配向角偏差角度亦可收斂至8~11°之範圍。 In Examples 5 to 9, the angle β at the measurement site was at most 9°, and it was found that a sintered body showing a radial alignment as designed was obtained by a deformation operation. Moreover, it can be confirmed that the situation of any embodiment, the maximum alignment axis angle difference Both are non-parallel alignments above 20°. Although the deviation of the alignment angle of the embodiment 9 is slightly larger, it is considered to be due to the difference in the alignment means. When the same apparatus as in the fourth to eighth embodiments is used, it is considered that the angle of deviation of the alignment angle of the embodiment 9 can also converge to a range of 8 to 11 degrees.

又，針對變形量最大之實施例9之燒結體，將該燒結體於長度方向中央切斷，藉由SEM觀察該剖面之龜裂深度並測定後，為35μm，可確認幾乎不產生龜裂。測定燒結後之磁石材料粒子之長寬比後，均為未達1.7。 In the sintered body of Example 9 having the largest amount of deformation, the sintered body was cut at the center in the longitudinal direction, and the crack depth of the cross section was observed by SEM and measured to be 35 μm, and it was confirmed that cracks were hardly generated. After measuring the aspect ratio of the magnet material particles after sintering, they were all less than 1.7.

表9中顯示個實施例之分析部位之數據。關於梯形形狀之實施例1~3，左側端部與相當於中央之分析位置之直線距離記為d，於該分析位置之配向角度差記為。進而於2點分析位置內，該分析位置中與最接近表面 之距離於表中表示為最近分析位置之距離。實施例4~9中，分析位置a與分析位置b之直線距離記為d，於其分析位置之配向角度差記為。進而於2點分析位置內，與最接近表面之距離於表中表示為最近分析位置之距離。 The data of the analysis sites of the examples are shown in Table 9. Regarding the first to third embodiments of the trapezoidal shape, the linear distance between the left end portion and the analysis position corresponding to the center is denoted by d, and the alignment angle difference at the analysis position is denoted as . Further, within the 2-point analysis position, the distance from the closest surface in the analysis position is expressed as the distance from the table to the nearest analysis position. In the fourth to ninth embodiments, the straight line distance between the analysis position a and the analysis position b is denoted by d, and the alignment angle difference at the analysis position is recorded as . Further, within the analysis point at 2 o'clock, the distance from the closest surface is expressed as the distance from the table to the nearest analysis position.

S-1‧‧‧第1表面 S-1‧‧‧ first surface

S-2‧‧‧第2表面 S-2‧‧‧ second surface

E-1、E-2‧‧‧端面 E-1, E-2‧‧‧ end face

B-1、B-2、B-3‧‧‧箭頭 B-1, B-2, B-3‧‧‧ arrows

B‧‧‧配向軸角度 B‧‧‧Alignment shaft angle

R‧‧‧4邊形區劃 R‧‧‧4 zoning

P‧‧‧磁石材料粒子 P‧‧‧Magnetic material particles

P-1‧‧‧易磁化軸 P-1‧‧‧Electronic axis

M‧‧‧稀土類磁石 M‧‧‧Rare Earth Magnet

W‧‧‧寬度 W‧‧‧Width

t‧‧‧厚度 T‧‧‧thickness

Claims (6)

一種稀土類磁石形成用燒結體，具有使含有稀土類物質之各具有易磁化軸之多數磁石材料粒子一體燒結之構成之稀土類磁石形成用燒結體，其特徵係：形成為具有長度方向之長度尺寸、於與該長度方向呈直角之橫方向之剖面中之於第1表面與第2表面間之厚度方向之厚度尺寸、對於該厚度方向正交之方向之厚度正交尺寸之立體形狀，具有於包含前述厚度方向與前述厚度正交方向之面內之任意位置之含有30個以上之前述磁石材料粒子之4角形區劃內之所有前述磁石材料粒子之各者之易磁化軸相對於預先決定之基準線之配向角中定義為頻率最高之配向角之配向軸角度差20°以上之至少2個區域，且基於前述區劃之各者中前述磁石材料粒子之各者之易磁化軸之配向角相對於前述配向軸角度之差而決定之配向角偏差角度為16.0°以下。 A sintered body for forming a rare earth magnet, which comprises a sintered body for forming a rare earth magnet which is formed by integrally sintering a plurality of magnet material particles each having a rare magnet material having an easy magnetization axis, and is characterized in that it has a length in the longitudinal direction. The dimension has a thickness dimension in a thickness direction between the first surface and the second surface in a cross section perpendicular to the longitudinal direction, and a three-dimensional shape having a thickness orthogonal to a direction perpendicular to the thickness direction. The easy magnetization axis of each of the magnet material particles in the quadrangular region including the magnet particles of 30 or more at any position in the plane including the thickness direction and the thickness orthogonal direction is determined in advance with respect to the predetermined The alignment angle of the reference line is defined as at least two regions having an alignment angle angle of the highest frequency of the alignment angle of at least two degrees, and the alignment angle of the easy magnetization axis of each of the magnet material particles in each of the regions is relatively The angle of deviation deviation determined by the difference in the angle of the alignment axis is 16.0° or less. 一種稀土類磁石形成用燒結體，具有使含有稀土類物質之各具有易磁化軸之多數磁石材料粒子一體燒結之構成之稀土類磁石形成用燒結體，其特徵係：形成為具有長度方向之長度尺寸、於與該長度方向呈直角之橫方向之剖面中之於第1表面與第2表面間之厚度方向之厚度尺寸、對於該厚度方向正交之方向之厚度正交尺寸之立體形狀，具有於包含前述厚度方向與前述厚度正交方向之面內 之任意位置之一邊為35μm之正方形區劃內之所有前述磁石材料粒子之各者之易磁化軸相對於預先決定之基準線之配向角中定義為頻率最高之配向角之配向軸角度差20°以上之至少2個區域，且基於前述區劃之各者中前述磁石材料粒子之各者之易磁化軸之配向角相對於前述配向軸角度之差而決定之配向角偏差角度為16.0°以下。 A sintered body for forming a rare earth magnet, which comprises a sintered body for forming a rare earth magnet which is formed by integrally sintering a plurality of magnet material particles each having a rare magnet material having an easy magnetization axis, and is characterized in that it has a length in the longitudinal direction. The dimension has a thickness dimension in a thickness direction between the first surface and the second surface in a cross section perpendicular to the longitudinal direction, and a three-dimensional shape having a thickness orthogonal to a direction perpendicular to the thickness direction. In the plane including the direction in which the thickness direction is orthogonal to the thickness Any one of the positions of any of the foregoing magnet material particles in a square region of 35 μm is a phase difference of 20° or more from an alignment axis of an alignment angle defined as a frequency with respect to a predetermined reference line. In at least two regions, the angle of deviation deviation determined by the difference in the alignment angle of the easy magnetization axis of each of the magnet material particles in each of the regions is 16.0° or less with respect to the difference in the angle of the alignment axis. 如請求項1或2之稀土類磁石形成用燒結體，其中前述磁石材料粒子之平均粒徑為3μm以下。 The sintered body for forming a rare earth magnet according to claim 1 or 2, wherein the magnet material particles have an average particle diameter of 3 μm or less. 如請求項1至3中任一項之稀土類磁石形成用燒結體，其中前述立體形狀係與前述長度方向為直角之橫方向之剖面成為梯形之形狀。 The sintered body for forming a rare earth magnet according to any one of claims 1 to 3, wherein the three-dimensional shape has a trapezoidal shape in a cross section perpendicular to the longitudinal direction. 如請求項1至3中任一項之稀土類磁石形成用燒結體，其中前述立體形狀係以具有前述第1表面及前述第2表面之兩者形成為具有相同曲率中心之圓弧形狀之圓弧狀剖面之方式，形成與前述長度方向為直角之橫方向之剖面。 The sintered body for forming a rare earth magnet according to any one of claims 1 to 3, wherein the three-dimensional shape is formed into a circle having an arc shape having the same center of curvature by both of the first surface and the second surface. In the form of an arc-shaped cross section, a cross section perpendicular to the longitudinal direction is formed. 一種稀土類燒結磁石，其係藉由使如請求項1至5中任一項之稀土類磁石形成用燒結體磁化而形成。 A rare earth sintered magnet which is formed by magnetizing a sintered body for forming a rare earth magnet according to any one of claims 1 to 5.
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